ࡱ>   U6 s u X lxlnprtvxz|~B D!!F""H##J$$L%%N&&P''R((T))V**X++Z,,\--l..I//01G11L22N33P44R55y& bjbj W{{  ddddd$X!|1$V@9F>>>.1L(#%%%%%%$<jIQ dc@Idd>>%|||d>d>#|#||v|>@r@g|0pdE*o|EEEIIZ"EEEEEEEEEEEE  *: SVEU ILI`TE U ZAGREBU RUDARSKO-GEOLO`KO-NAFTNI FAKULTET Irma Belamari TERMODINAMI KA KARAKTERIZACIJA UGLJIKOVODIKA JEDINSTVENOM JEDNAD}BOM STANJA I PRI TEMPERATURAMA RAZLI ITIM OD LE}I`NE DOKTORSKI RAD Zagreb, 2012.  UNIVERSITY OF ZAGREB FACULTY OF MINING, GEOLOGY AND PETROLEUM ENGINEERING Irma Belamari THERMODYNAMIC CHARACTERIZATION OF HYDROCARBONS BY SINGLE EQUATION OF STATE AND AT TEMPERATURES DIFFERENT FROM THE RESERVOIR TEMPERATURE DOCTORAL THESIS Zagreb, 2012  SVEU ILI`TE U ZAGREBU RUDARSKO-GEOLO`KO-NAFTNI FAKULTET IRMA BELAMARI TERMODINAMI KA KARAKTERIZACIJA UGLJIKOVODIKA JEDINSTVENOM JEDNAD}BOM STANJA I PRI TEMPERATURAMA RAZLI ITIM OD LE}I`NE DOKTORSKI RAD Mentor: dr. sc. Domagoj Vulin, docent Rudarsko-geoloako-naftnog fakulteta Zagreb, 2012. Doktorski rad sadr~i: Broj stranica teksta: 151 Broj slika u tekstu: 81 Broj tablica u tekstu: 33 Broj priloga: 4 Broj literaturnih navoda: 104 ZAHVALA Prvenstveno se zahvaljujem mentoru dr. sc. Domagoju Vulinu na ulo~enom trudu, strpljenju te korisnim raspravama i kriti kim uputama koje su oblikovale ovaj rad. Zahvaljujem se lanovima povjerenstva: dr. sc. Tomislavu Kureviji, dr. sc. Frankici Kapor, dr. sc. Sanji Martinez i dr. sc. Mariu `avaru na stru noj pomoi i recenziji ovog rada. Posebno se zahvaljujem pokojnom profesoru Bogdanu Gori niku na zaraznom entuzijazmu prema poslu koji radim te njegovom izuzetnom znanju kojeg je tek dio uspio prenijeti i na mene. Iskreno hvala mojim najbli~im kolegama iz naaeg PVT laboratorija: Mirjani, Slavici ., Slavici M., Damiru, Jo~i, Siniai, Darku, Stjepanu, Marku i Saai. Takoer se zahvaljujem svim ostalim kolegama iz Slu~be laboratorijskih ispitivanja IPNP, posebice Zdenkici, Tamari i Morani. Najvee hvala mojim kolegicama, stru njacima, ali prije svega pravim i iskrenim prijateljicama Snje~ani i Jasmini. Zahvaljujem se i svojoj kompaniji INA d.d. na ukazanom povjerenju i financijskoj potpori tijekom doktorskog studija. Na kraju se zahvaljujem cijeloj svojoj obitelji na pru~anoj podraci, a posebno suprugu Tomi na strpljenju i svoj moguoj potpori tijekom izrade rada. Doktorski rad posveujem svojim princezama Petri i Korini. SA}ETAK U praksi laboratorijskih analiza ugljikovodika iz le~iata nafte i plina uobi ajeno je raditi eksperimente pri le~ianoj temperaturi. Kona ni rezultat analize jest izvjeataj o termodinami kim (PVT) odnosima i jednad~ba stanja podeaena za svaki specifi ni fluid iz le~iata, a u svrhu predikcije budue proizvodnje te planiranja metode eksploatacije. Ograni enja i manjkavosti ovakve metode su prije svega visoke temperature pri kojima laboratorijske analize postaju neizvedive (T>200C), kao i razlike u sastavima fluida unutar jedne hidrodinami ke cjeline tj. le~iata. Laboratorijske analize raene blizu kriti ne to ke fluida (npr. ako je temperatura le~iata blizu kriti ne temperature fluida) u pravilu dovode do neegzaktnog PVT modela. Nova eksperimentalna metoda te druga iji pristup podeaavanja parametara jednad~be stanja omoguili bi to niji kona ni rezultat te jedinstvenu jednad~bu stanja koja bi opisivala fluid u cijelom volumenu le~iata, a ne samo analizirani uzorak iz pojedine buaotine. Klju ne rije i: PVT, laboratorijske analize, termodinami ka karakterizacija, jednad~ba stanja, gradijent sastava, visokotemperaturna le~iata SUMMARY Laboratory analyses of hydrocarbons from oil and gas reservoirs are commonly conducted at reservoir temperature. The final result of the analyses is the report that contains thermodynamic (PVT) data and the equation of state matched for each specific fluid from the reservoir. A PVT study is done in order to anticipate future production and to plan methods of exploitation. The limitations and shortcomings of this method are extremely high reservoir temperatures at which laboratory analyses become impracticable (T>200C), as well as differences in the composition of the fluid within the hydrodynamic unit, i.e. reservoir. A PVT model can also be imprecise if the laboratory analysis is done near the critical point of the fluid. A new experimental method and a different approach of adjusting equation of state parameters would provide a more accurate and a unique equation of state which would describe the entire volume of fluid in the reservoir, not only the analyzed samples from individual wells. Key words: PVT, laboratory analyses, thermodynamic characterization, equation of state, compositional gradient, high-temperature reservoirs SADR}AJ  TOC \o "1-4" \h \z \u  HYPERLINK \l "_Toc340820977" 1. UVOD  PAGEREF _Toc340820977 \h 1  HYPERLINK \l "_Toc340820978" 1.1. Postupak istra~ivanja  PAGEREF _Toc340820978 \h 3  HYPERLINK \l "_Toc340820979" 1.2. Pregled dosadaanjih istra~ivanja  PAGEREF _Toc340820979 \h 3  HYPERLINK \l "_Toc340820980" 2. TEORIJSKO RAZMATRANJE  PAGEREF _Toc340820980 \h 6  HYPERLINK \l "_Toc340820981" 2.1. Definiranje osnovnih pojmova i veli ina koji se koriste u opisu faznog ponaaanja le~ianih fluida  PAGEREF _Toc340820981 \h 6  HYPERLINK \l "_Toc340820982" 2.2. Laboratorijska termodinami ka karakterizacija le~ianih fluida  PAGEREF _Toc340820982 \h 13  HYPERLINK \l "_Toc340820983" 2.2.1 Uzorkovanje  PAGEREF _Toc340820983 \h 14  HYPERLINK \l "_Toc340820984" 2.2.2 Kontrola kvalitete uzoraka  PAGEREF _Toc340820984 \h 20  HYPERLINK \l "_Toc340820985" 2.2.3 PVT testovi  PAGEREF _Toc340820985 \h 21  HYPERLINK \l "_Toc340820986" 2.2.3.1 Analiza sastava i svojstava plina i nafte/kondenzata  PAGEREF _Toc340820986 \h 21  HYPERLINK \l "_Toc340820987" 2.2.3.2 Kontaktno otplinjavanje (flash) separatorske nafte/kondenzata  PAGEREF _Toc340820987 \h 24  HYPERLINK \l "_Toc340820988" 2.2.3.3 Rekombinacija le~ianog fluida  PAGEREF _Toc340820988 \h 28  HYPERLINK \l "_Toc340820989" 2.2.3.4 Test ekspanzije pri stalnom sastavu  PAGEREF _Toc340820989 \h 29  HYPERLINK \l "_Toc340820990" 2.2.3.5 Diferencijalno otparavanje  PAGEREF _Toc340820990 \h 30  HYPERLINK \l "_Toc340820991" 2.2.3.6 Separator test  PAGEREF _Toc340820991 \h 31  HYPERLINK \l "_Toc340820992" 2.2.3.7 Viskoznost  PAGEREF _Toc340820992 \h 32  HYPERLINK \l "_Toc340820993" 2.2.3.8 Test otparavanja pri stalnom volumenu  PAGEREF _Toc340820993 \h 32  HYPERLINK \l "_Toc340820994" 2.2.4 Procjena nesigurnosti termodinami kih parametara  PAGEREF _Toc340820994 \h 39  HYPERLINK \l "_Toc340820995" 2.2.4.1 To nost eksperimentalnih PVT podataka  PAGEREF _Toc340820995 \h 39  HYPERLINK \l "_Toc340820996" 2.3. Karakterizacija C7+ frakcije  PAGEREF _Toc340820996 \h 43  HYPERLINK \l "_Toc340820997" 2.3.1 Laboratorijska karakterizacija C7+ frakcije  PAGEREF _Toc340820997 \h 43  HYPERLINK \l "_Toc340820998" 2.3.2 Metode karakterizacije psudokomponenti za primjenu jednad~bi stanja  PAGEREF _Toc340820998 \h 45  HYPERLINK \l "_Toc340820999" 2.3.2.1 Matemati ki modeli molarne distribucije  PAGEREF _Toc340820999 \h 50  HYPERLINK \l "_Toc340821000" 2.4. Jednad~ba stanja  PAGEREF _Toc340821000 \h 56  HYPERLINK \l "_Toc340821001" 2.4.1 Povijesni razvoj jednad~bi stanja  PAGEREF _Toc340821001 \h 56  HYPERLINK \l "_Toc340821002" 2.4.2 Kubne jednad~be stanja  PAGEREF _Toc340821002 \h 57  HYPERLINK \l "_Toc340821003" 2.4.3 Jednad~ba stanja le~ianih ugljikovodi nih fluida  PAGEREF _Toc340821003 \h 64  HYPERLINK \l "_Toc340821004" 2.4.4 Podeaavanje parametara jednad~be stanja  PAGEREF _Toc340821004 \h 65  HYPERLINK \l "_Toc340821005" 2.4.4.1 Parametri regresije  PAGEREF _Toc340821005 \h 66  HYPERLINK \l "_Toc340821006" 2.5. Obrada podataka istra~ivanja  PAGEREF _Toc340821006 \h 74  HYPERLINK \l "_Toc340821007" 2.5.1 Statisti ka obrada podataka  PAGEREF _Toc340821007 \h 74  HYPERLINK \l "_Toc340821008" 2.5.2 Grafi ka obrada podataka  PAGEREF _Toc340821008 \h 76  HYPERLINK \l "_Toc340821009" 3. EKSPERIMENTALNO ISTRA}IVANJE  PAGEREF _Toc340821009 \h 77  HYPERLINK \l "_Toc340821010" 3.1. Uzorci  PAGEREF _Toc340821010 \h 77  HYPERLINK \l "_Toc340821011" 3.2. Instrumentacija i programska podraka  PAGEREF _Toc340821011 \h 81  HYPERLINK \l "_Toc340821012" 4. REZULTATI ISTRA}IVANJA  PAGEREF _Toc340821012 \h 94  HYPERLINK \l "_Toc340821013" 4.1. Provjera podataka koji prethode laboratorijskim PVT ispitivanjima  PAGEREF _Toc340821013 \h 94  HYPERLINK \l "_Toc340821014" 4.2. Podaci laboratorijskih PVT ispitivanja i njihova provjera  PAGEREF _Toc340821014 \h 103  HYPERLINK \l "_Toc340821015" 4.2.1 Maseno uravnote~enje separator testa  PAGEREF _Toc340821015 \h 104  HYPERLINK \l "_Toc340821016" 4.2.2 Materijalno uravnote~enje testa diferencijalnog otparavanja  PAGEREF _Toc340821016 \h 105  HYPERLINK \l "_Toc340821017" 4.2.3 Materijalno uravnote~enje testa otparavanja pri stalnom volumenu  PAGEREF _Toc340821017 \h 106  HYPERLINK \l "_Toc340821018" 4.2.4 Provjere analiza sastava tijekom testova otparavanja  PAGEREF _Toc340821018 \h 107  HYPERLINK \l "_Toc340821019" 4.3. Podeavanje parametara jednad~bi stanja na izabrane uzorke  PAGEREF _Toc340821019 \h 110  HYPERLINK \l "_Toc340821020" 4.3.1 Postupak podeaavanja parametara i provjera kvalitete jednad~be stanja na jednom uzorku le~ianog fluida  PAGEREF _Toc340821020 \h 111  HYPERLINK \l "_Toc340821021" 4.3.2 Usporedba rezultata jednad~be stanja podeaene na viae uzoraka s rezultatima jednad~bi stanja podeaenih na pojedina nim uzorcima  PAGEREF _Toc340821021 \h 120  HYPERLINK \l "_Toc340821022" 4.4. Rezultati termodinami kih ispitivanja provedenih pri temperaturama razli itim od le~iane temperature  PAGEREF _Toc340821022 \h 134  HYPERLINK \l "_Toc340821023" 4.5. Procedure termodinami ke karakterizacije le~ianih fluida  PAGEREF _Toc340821023 \h 146  HYPERLINK \l "_Toc340821024" 4.5.1 Preporu ena procedura termodinami ke karakterizacije jednog uzorka  PAGEREF _Toc340821024 \h 146  HYPERLINK \l "_Toc340821025" 4.5.2 Preporu ena procedura termodinami ke karakterizacije viae uzoraka  PAGEREF _Toc340821025 \h 149  HYPERLINK \l "_Toc340821026" 5. ZAKLJU AK  PAGEREF _Toc340821026 \h 150  HYPERLINK \l "_Toc340821027" 6. LITERATURA  PAGEREF _Toc340821027 \h 152  POPIS TABLICA U TEKSTU  TOC \h \z \c "Tablica"  HYPERLINK \l "_Toc335391083" Tablica 21. Tipi ni sastavi i svojstva razli itih tipova le~ianih fluida (Whitson & Brul, 2000)  PAGEREF _Toc335391083 \h 7  HYPERLINK \l "_Toc335391084" Tablica 22. To nost eksperimentalnih podataka  PAGEREF _Toc335391084 \h 41  HYPERLINK \l "_Toc335391085" Tablica 23. Fizikalna svojstva ugljikovodi nih frakcija  PAGEREF _Toc335391085 \h 47  HYPERLINK \l "_Toc335391086" Tablica 24. Koeficijenti jednad~be 2-25 (Ahmed et al., 1985)  PAGEREF _Toc335391086 \h 48  HYPERLINK \l "_Toc335391087" Tablica 25. Nulto ke i te~ine za prvih 5 Laguerreovih polinoma (Abramowitz & Stegun, 1965)  PAGEREF _Toc335391087 \h 53  HYPERLINK \l "_Toc335391088" Tablica 26. Prekretnice u razvoju jednad~be stanja  PAGEREF _Toc335391088 \h 57  HYPERLINK \l "_Toc335391089" Tablica 27. Preporu eni binarni interakcijski parametri za Peng-Robinsonovu i Soave-Redlich-Kwongovu jednad~ba stanja  PAGEREF _Toc335391089 \h 63  HYPERLINK \l "_Toc335391090" Tablica 28. Parametri volumnog pomaka istih komponenata za PR JS i SRK JS (Whitson i Brul, 2000)  PAGEREF _Toc335391090 \h 64  HYPERLINK \l "_Toc335391091" Tablica 29. Koeficijenti za Riazi-Daubertovu korelaciju (Riazi & Daubert, 1980)  PAGEREF _Toc335391091 \h 69  HYPERLINK \l "_Toc335391092" Tablica 31. Izvrene analize  PAGEREF _Toc335391092 \h 78  HYPERLINK \l "_Toc335391093" Tablica 32. Temperaturni program metode za analizu plinske faze  PAGEREF _Toc335391093 \h 82  HYPERLINK \l "_Toc335391094" Tablica 33. Temperaturni program metode za analizu tekueg ugljikovodi nog fluida  PAGEREF _Toc335391094 \h 84  HYPERLINK \l "_Toc335391095" Tablica 34. Dijeljenje C7+ frakcije modificiranom Whitsonovom metodom (1989)  PAGEREF _Toc335391095 \h 92  HYPERLINK \l "_Toc335391096" Tablica 41. Podaci za C7+ frakcije analiziranih uzoraka. Izabrani reprezentativni uzorci za pojedino polje su osjen ani.  PAGEREF _Toc335391096 \h 95  HYPERLINK \l "_Toc335391097" Tablica 42. Prora un materijalnog uravnote~enja promatranog uzorka tijekom testa diferencijalnog otparavanja  PAGEREF _Toc335391097 \h 106  HYPERLINK \l "_Toc335391098" Tablica 43. Pregled postupka podeaavanja parametara jednad~be stanja po koracima  PAGEREF _Toc335391098 \h 111  HYPERLINK \l "_Toc335391099" Tablica 44. Parametri kona ne (korak br. 9) podeaene jednad~be stanja  PAGEREF _Toc335391099 \h 113  HYPERLINK \l "_Toc335391100" Tablica 45. Binarni interakcijski parametri  PAGEREF _Toc335391100 \h 113  HYPERLINK \l "_Toc335391101" Tablica 46. Usporedba rezultata separatorskog testa po koracima  PAGEREF _Toc335391101 \h 115  HYPERLINK \l "_Toc335391102" Tablica 47. Parametri jednad~be stanja JS 1  PAGEREF _Toc335391102 \h 121  HYPERLINK \l "_Toc335391103" Tablica 48. Binarni interakcijski parametri za JS 1  PAGEREF _Toc335391103 \h 121  HYPERLINK \l "_Toc335391104" Tablica 49. Parametri jednad~be stanja JS 2  PAGEREF _Toc335391104 \h 122  HYPERLINK \l "_Toc335391105" Tablica 410. Binarni interakcijski parametri za JS 2  PAGEREF _Toc335391105 \h 122  HYPERLINK \l "_Toc335391106" Tablica 411. Parametri jednad~be stanja JS 3  PAGEREF _Toc335391106 \h 123  HYPERLINK \l "_Toc335391107" Tablica 412. Binarni interakcijski parametri za JS 3  PAGEREF _Toc335391107 \h 123  HYPERLINK \l "_Toc335391108" Tablica 413. Usporedba rezultata separator testa  PAGEREF _Toc335391108 \h 125  HYPERLINK \l "_Toc335391109" Tablica 414. Izra unati i eksperimentalno odreeni tlakovi zasienja  PAGEREF _Toc335391109 \h 136  HYPERLINK \l "_Toc335391110" Tablica 415. Odstupanja tlakova zasienja izra unatih pojedinim jednad~bama stanja u odnosu na eksperimentalno odreene vrijednosti  PAGEREF _Toc335391110 \h 137  HYPERLINK \l "_Toc335391111" Tablica 416. Statisti ka obrada udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu pri 35C reproduciranog pojedinim jednad~bama stanja  PAGEREF _Toc335391111 \h 143  HYPERLINK \l "_Toc335391112" Tablica 417. Statisti ka obrada udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi (119C) reproduciranog pojedinim jednad~bama stanja  PAGEREF _Toc335391112 \h 143  HYPERLINK \l "_Toc335391113" Tablica 418. Volumeni retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu provedenog pri 119C reproduciranog pojedinim jednad~bama stanja  PAGEREF _Toc335391113 \h 144  HYPERLINK \l "_Toc335391114" Tablica 419. Relativna odstupanja volumena retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu provedenog pri 119C reproduciranog pojedinim jednad~bama stanja  PAGEREF _Toc335391114 \h 145  HYPERLINK \l "_Toc335391115" Tablica 420. Statisti ka obrada rezultata testa otparavanja pri stalnom volumenu provedenog pri 119C reproduciranog pojedinim jednad~bama stanja  PAGEREF _Toc335391115 \h 145  POPIS SLIKA U TEKSTU  TOC \h \z \c "Slika"  HYPERLINK \l "_Toc340748586" Slika 21. Fazni dijagram suhog plina  PAGEREF _Toc340748586 \h 9  HYPERLINK \l "_Toc340748587" Slika 22. Fazni dijagram mokrog plina  PAGEREF _Toc340748587 \h 10  HYPERLINK \l "_Toc340748588" Slika 23. Fazni dijagram plinskog kondenzata  PAGEREF _Toc340748588 \h 11  HYPERLINK \l "_Toc340748589" Slika 24. Fazni dijagram hlapive nafte  PAGEREF _Toc340748589 \h 11  HYPERLINK \l "_Toc340748590" Slika 25. Fazni dijagram nafte  PAGEREF _Toc340748590 \h 12  HYPERLINK \l "_Toc340748591" Slika 26. Dijagram tijeka laboratorijskog ispitivanja naftnih le~ianih fluida  PAGEREF _Toc340748591 \h 13  HYPERLINK \l "_Toc340748592" Slika 27. Dijagram tijeka laboratorijskog ispitivanja plinsko kondenzatnih le~ianih fluida  PAGEREF _Toc340748592 \h 14  HYPERLINK \l "_Toc340748593" Slika 28. Uzorkovanje separatorskog plina i nafte (INA, 2003)  PAGEREF _Toc340748593 \h 15  HYPERLINK \l "_Toc340748594" Slika 29. Uzorkovanje dubinskog uzorka le~ianog fluida (INA, 2003)  PAGEREF _Toc340748594 \h 15  HYPERLINK \l "_Toc340748595" Slika 210. Kromatogram uzorka prirodnog plina  PAGEREF _Toc340748595 \h 22  HYPERLINK \l "_Toc340748596" Slika 211. Analiza nafte na plinskom kromatografu Agilent Technologies 6890N  PAGEREF _Toc340748596 \h 23  HYPERLINK \l "_Toc340748597" Slika 212. Shematski prikaz testa ekspanzije nafte  PAGEREF _Toc340748597 \h 29  HYPERLINK \l "_Toc340748598" Slika 213. Shematski prikaz testa diferencijalnog otparavanja  PAGEREF _Toc340748598 \h 31  HYPERLINK \l "_Toc340748599" Slika 214. Shematski prikaz testa vie stupanjske separacije nafte (Whitson & Brul, 2000)  PAGEREF _Toc340748599 \h 32  HYPERLINK \l "_Toc340748600" Slika 215. Shematski prikaz testa otparavanja pri stalnom volumenu (Gori nik, 2006)  PAGEREF _Toc340748600 \h 33  HYPERLINK \l "_Toc340748601" Slika 216. Primjer provjere K-omjera (Martinsen et al., 2010)  PAGEREF _Toc340748601 \h 38  HYPERLINK \l "_Toc340748602" Slika 217. Krivulja simulirane destilacije  PAGEREF _Toc340748602 \h 44  HYPERLINK \l "_Toc340748603" Slika 218. Distribucija frakcija jedinstvenog uglji nog broja odreenih metodom plinske kromatografije na uzorku kondenzata  PAGEREF _Toc340748603 \h 45  HYPERLINK \l "_Toc340748604" Slika 219. Grafi ki prikaz utjecaja razli itih korelacija na predvianje jednad~be stanja (Whitson, 1984)  PAGEREF _Toc340748604 \h 46  HYPERLINK \l "_Toc340748605" Slika 220. Molni udio dobiven razlikom povraina ispod funkcije gustoe vjerojatnosti unutar odreenih molnih udjela (Sreide, 1989)  PAGEREF _Toc340748605 \h 51  HYPERLINK \l "_Toc340748606" Slika 221. Acentri ni faktor (Gori nik, 2006)  PAGEREF _Toc340748606 \h 60  HYPERLINK \l "_Toc340748607" Slika 31. PVT spremnici sa separatorskim uzorcima  PAGEREF _Toc340748607 \h 77  HYPERLINK \l "_Toc340748608" Slika 32. Plinski kromatograf za analizu plinske faze  PAGEREF _Toc340748608 \h 82  HYPERLINK \l "_Toc340748609" Slika 33. Plinski kromatograf za analizu tekue faze  PAGEREF _Toc340748609 \h 84  HYPERLINK \l "_Toc340748610" Slika 34. Kontaktno otplinjavanje separatorske nafte  PAGEREF _Toc340748610 \h 85  HYPERLINK \l "_Toc340748611" Slika 35. elija za rekombinaciju  PAGEREF _Toc340748611 \h 86  HYPERLINK \l "_Toc340748612" Slika 36. Instrument 3000 PVT Phase Behavior System  PAGEREF _Toc340748612 \h 87  HYPERLINK \l "_Toc340748613" Slika 37. Instrument za provedbu separator testa model 2353-805 Equilibrium Flash Separator  PAGEREF _Toc340748613 \h 88  HYPERLINK \l "_Toc340748614" Slika 38. Shematski prikaz viskozimetra s rotirajuom kuglicom  PAGEREF _Toc340748614 \h 89  HYPERLINK \l "_Toc340748615" Slika 41. Grafi ki prikaz molarne mase u odnosu na relativnu gustou C7+ frakcija analiziranih uzoraka  PAGEREF _Toc340748615 \h 95  HYPERLINK \l "_Toc340748616" Slika 42. Grafi ki prikaz Watsonovog karakterizacijskog faktora analiziranih uzoraka  PAGEREF _Toc340748616 \h 96  HYPERLINK \l "_Toc340748617" Slika 43. Provjera Watsonovog karakterizacijskog faktora za polje A  PAGEREF _Toc340748617 \h 96  HYPERLINK \l "_Toc340748618" Slika 44. Provjera Watsonovog karakterizacijskog faktora za polje B  PAGEREF _Toc340748618 \h 97  HYPERLINK \l "_Toc340748619" Slika 45. Provjera Watsonovog karakterizacijskog faktora za polje C  PAGEREF _Toc340748619 \h 97  HYPERLINK \l "_Toc340748620" Slika 46. Provjera kvalitete sastava uzorka A-2-9: odnos molnog udjela na log skali i jedinstvenih uglji nih brojeva  PAGEREF _Toc340748620 \h 98  HYPERLINK \l "_Toc340748621" Slika 47. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka A-2-17  PAGEREF _Toc340748621 \h 98  HYPERLINK \l "_Toc340748622" Slika 48. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka A-1-2  PAGEREF _Toc340748622 \h 99  HYPERLINK \l "_Toc340748623" Slika 49. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka E-2-3  PAGEREF _Toc340748623 \h 99  HYPERLINK \l "_Toc340748624" Slika 410. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka C-3-1  PAGEREF _Toc340748624 \h 100  HYPERLINK \l "_Toc340748625" Slika 411. Grafi ki prikaz HCH/Standing korelacije za uzorak A-2-9  PAGEREF _Toc340748625 \h 100  HYPERLINK \l "_Toc340748626" Slika 412. Grafi ki prikaz HCH/Standing korelacije za uzorak A-2-17  PAGEREF _Toc340748626 \h 101  HYPERLINK \l "_Toc340748627" Slika 413. Grafi ki prikaz HCH/Standing korelacije za uzorak C-3-1  PAGEREF _Toc340748627 \h 101  HYPERLINK \l "_Toc340748628" Slika 414. Grafi ki prikaz HCH/Standing korelacije za uzorak E-2-3  PAGEREF _Toc340748628 \h 102  HYPERLINK \l "_Toc340748629" Slika 415. Grafi ki prikaz HCH/Standing korelacije za uzorak A-1-2  PAGEREF _Toc340748629 \h 102  HYPERLINK \l "_Toc340748630" Slika 416. Grafi ki prikaz komponentnog sastava plinova proizvedenih tijekom otparavanja pri stalnom volumenu za uzorak A-2-9  PAGEREF _Toc340748630 \h 108  HYPERLINK \l "_Toc340748631" Slika 417. Grafi ki prikaz dvofaznog Z faktora tijekom otparavanja pri stalnom volumenu za uzorak A-2-9  PAGEREF _Toc340748631 \h 108  HYPERLINK \l "_Toc340748632" Slika 418. Grafi ki prikaz komponentnog sastava tekue faze (xi) na logaritamskoj skali u odnosu na tlak otparavanja za uzorak A-2-9  PAGEREF _Toc340748632 \h 109  HYPERLINK \l "_Toc340748633" Slika 419. Grafi ki prikaz K omjera na logaritamskoj skali u odnosu na tlak otparavanja za uzorak A-2-9  PAGEREF _Toc340748633 \h 109  HYPERLINK \l "_Toc340748634" Slika 420. Prikaz faznih dijagrama svih verzija jednad~be stanja  PAGEREF _Toc340748634 \h 114  HYPERLINK \l "_Toc340748635" Slika 421. Grafi ki prikaz rezultata separator testa po koracima - proizvodni plinski faktor  PAGEREF _Toc340748635 \h 116  HYPERLINK \l "_Toc340748636" Slika 422. Grafi ki prikaz rezultata separator testa po koracima - gustoa tekue faze  PAGEREF _Toc340748636 \h 116  HYPERLINK \l "_Toc340748637" Slika 423. Grafi ka usporedba rezultata testa ekspanzije pri stalnom sastavu - volumni faktor nafte  PAGEREF _Toc340748637 \h 117  HYPERLINK \l "_Toc340748638" Slika 424. Grafi ka usporedba rezultata testa ekspanzije pri stalnom sastavu - relativni volumen  PAGEREF _Toc340748638 \h 117  HYPERLINK \l "_Toc340748639" Slika 425. Grafi ka usporedba proizvodnog plinskog faktora tijekom testa diferencijalnog otparavanja  PAGEREF _Toc340748639 \h 118  HYPERLINK \l "_Toc340748640" Slika 426. Grafi ka usporedba gustoe nafte tijekom testa diferencijalnog otparavanja  PAGEREF _Toc340748640 \h 118  HYPERLINK \l "_Toc340748641" Slika 427. Grafi ka usporedba volumnog faktora nafte tijekom testa diferencijalnog otparavanja  PAGEREF _Toc340748641 \h 119  HYPERLINK \l "_Toc340748642" Slika 428. Grafi ki prikaz faznih krivulja izra unatih s tri jednad~be stanja  PAGEREF _Toc340748642 \h 124  HYPERLINK \l "_Toc340748643" Slika 429. Grafi ki prikaz relativnih volumena plinskog kondenzata tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  PAGEREF _Toc340748643 \h 125  HYPERLINK \l "_Toc340748644" Slika 430. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  PAGEREF _Toc340748644 \h 126  HYPERLINK \l "_Toc340748645" Slika 431. Grafi ki prikaz relativnih volumena nafte tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  PAGEREF _Toc340748645 \h 126  HYPERLINK \l "_Toc340748646" Slika 432. Grafi ki prikaz volumnih faktora nafte tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  PAGEREF _Toc340748646 \h 127  HYPERLINK \l "_Toc340748647" Slika 433. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu s tri jednad~be stanja  PAGEREF _Toc340748647 \h 127  HYPERLINK \l "_Toc340748648" Slika 434. Grafi ki prikaz Z faktora plina tijekom testa otparavanja pri stalnom volumenu s tri jednad~be stanja  PAGEREF _Toc340748648 \h 128  HYPERLINK \l "_Toc340748649" Slika 435. Grafi ki prikaz volumnih faktora nafte tijekom testa diferencijalnog otparavanja s tri jednad~be stanja  PAGEREF _Toc340748649 \h 128  HYPERLINK \l "_Toc340748650" Slika 436. Grafi ki prikaz proizvodnog plinskog faktora tijekom testa diferencijalnog otparavanja s tri jednad~be stanja  PAGEREF _Toc340748650 \h 129  HYPERLINK \l "_Toc340748651" Slika 437. Grafi ki prikaz gustoe nafte tijekom testa diferencijalnog otparavanja sa tri jednad~be stanja  PAGEREF _Toc340748651 \h 129  HYPERLINK \l "_Toc340748652" Slika 438. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu za uzorak A-6-2 (plinski kondenzat)  PAGEREF _Toc340748652 \h 130  HYPERLINK \l "_Toc340748653" Slika 439. Grafi ki prikaz plinskog faktora tijekom testa diferencijalnog otparavanja za uzorak A-2-13 (nafta)  PAGEREF _Toc340748653 \h 131  HYPERLINK \l "_Toc340748654" Slika 440. Fazni dijagrami reproducirani jedinstvenom jednad~bom stanja  PAGEREF _Toc340748654 \h 131  HYPERLINK \l "_Toc340748655" Slika 441. Fazni dijagrami reproducirani jedinstvenom jednad~bom stanja  PAGEREF _Toc340748655 \h 132  HYPERLINK \l "_Toc340748656" Slika 442. Udio retrogradne kondenzacije tijekom testa otparavanja pri stalnom volumenu reproduciran jedinstvenom jednad~bom stanja  PAGEREF _Toc340748656 \h 133  HYPERLINK \l "_Toc340748657" Slika 443. Grafi ki prikaz tlakova zasienja u rasponu temperatura od 20C do 200C reproduciranih razli itim jednad~bama stanja  PAGEREF _Toc340748657 \h 135  HYPERLINK \l "_Toc340748658" Slika 444. Grafi ki prikaz gustoa pri tlakovima zasienja u rasponu temperatura od 20C do 200C reproduciranih razli itim jednad~bama stanja  PAGEREF _Toc340748658 \h 136  HYPERLINK \l "_Toc340748659" Slika 445. Grafi ki prikaz relativnih odstupanja izra unatih tlakova zasienja u odnosu na eksperimentalno odreene vrijednosti tlaka zasienja  PAGEREF _Toc340748659 \h 138  HYPERLINK \l "_Toc340748660" Slika 446. Grafi ki prikaz udjela retrogradnog kondenzata tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748660 \h 139  HYPERLINK \l "_Toc340748661" Slika 447. Grafi ki prikaz relativnog volumena tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748661 \h 139  HYPERLINK \l "_Toc340748662" Slika 448. Grafi ki prikaz Z faktora plina tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748662 \h 140  HYPERLINK \l "_Toc340748663" Slika 449. Grafi ki prikaz udjela retrogradnog kondenzata tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748663 \h 141  HYPERLINK \l "_Toc340748664" Slika 450. Grafi ki prikaz relativnog volumena tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748664 \h 141  HYPERLINK \l "_Toc340748665" Slika 451. Grafi ki prikaz Z faktora plina tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748665 \h 142  HYPERLINK \l "_Toc340748666" Slika 452. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu pri 119C i reproduciranog razli itim jednad~bama stanja  PAGEREF _Toc340748666 \h 145  POPIS PRILOGA: PRILOG I Eksperimentalni podaci PRILOG II Podaci PVT testova reproduciranih jednad~bama stanja podeaenim pri razli itim temperaturama PRILOG III }ivotopis autora PRILOG IV Popis objavljenih radova autora NOMENKLATURA API - gustoa izra~ena u API B - volumni faktor, m3/m3 B(T), C(T), D(T),& - virijalni koeficijenti Bg - volumni faktor plina,m3/m3 bi - konstanta komponente i (jednad~ba 2-6) Bo - volumni faktor nafte, m3/m3 c - koeficijent stla ivosti fluida, bar-1 C1, C2, C3, C4, C5, C6, C7 - metan, etan, propan, butan, pentan, heksan, heptan ci - koeficijent volumnog pomaka komponente i GOR - plinski faktor, m3/m3 Hg - ~iva K - K-omjer, ravnote~ni omjer Ki - K-omjer, ravnote~ni omjer komponente i Kw - Watsonov faktor karakterizacije m - koeficijent jednad~be stanja MC7+ - molarna masa komponente C7+, g/mol Mi - molarna masa komponente i, g/mol n - koli ina tvari, mol p - tlak, bar p(M) - funkcija gustoe vjerojatnosti pb - tlak isparavanja, bar pc - kriti ni tlak, bar pcp - kriti ni tlak normalnih parafina, bar pd - tlak rosiata, bar ps - tlak zasienja, bar R - univerzalna plinska konstanta (=8,3143), Jmol-1K-1  EMBED Equation.3  - kvadratna sredina rezidualnih odstupanja ri - rezidualno odstupanje vrijednosti i Rs - faktor otopljenog plina, m3/m3 Tb - temperatura vrenja (vreliate), K Tc - kriti na temperatura, K Tcp - kriti na temperatura normalnih parafina, K Tr - reducirana temperatura Tsep - temperatura separacije (separatora), C Vc - kriti ni molarni volumen, m3/mol Vcp - kriti ni molarni volumen normalnih parafina, m3/mol Vgsc - volumen plinske faze pri standardnim uvjetima, m3 VL - volumen tekue faze, m3 Vliq - postotni udio volumena retrogradnog kondenzata, % Vm - molarni volumen plina, m3/mol VmL - nekorigirani molarni volumen tekue faze, m3/mol VmLcorr - korigirani molarni volumen tekue faze, m3/mol Vosep - volumen nafte pri separatorskim uvjetima, m3 Vrel - relativni volumen fluida, m3/m3 wi - ponderacijski faktor woi - te~ine iz Laguerreovih polinoma xi - koncentracija, izra~ena molnim udjelom komponente u tekuoj fazi xoi - nulto ke iz Laguerreovih polinoma yic - izra unata vrijednost opa~anja i yie - eksperimentalna vrijednost opa~anja i yir - referentna vrijednost opa~anja i Z - faktor kompresibilnosti plina zC7+ - molarni udio C7+ frakcije Zd - faktor kompresibilnosti plina pri tlaku rosita Zdvofazni - dvofazni Z faktor zi - molarni udio komponente i ( - fizikalno svojstvo ( - standardna devijacija ((() - gama funkcija (2 - zbroj kvadrata ponderiranih rezidualnih odstupanja (i - standardna devijacija opa~anja i  - bezdimenzionalni faktor u jednad~bama stanja , ,  - parametri koji definiraju molarnu distribuciju  - koeficijent termi ke ekspanzije, C-1 mjer - izmjerena varijabla pred - izra unata varijabla  - acentri ni faktor A - koeficijent jednad~be stanja B - koeficijent jednad~be stanja g - relativna gustoa gC7+ - relativna gustoa C7+ frakcije go - relativna gustoa nafte gp - relativna gustoa normalnih parafina m - viskoznost (mPas) UVOD Laboratorijska ispitivanja termodinami kih svojstava le~ianih fluida zapo inju uzorkovanjem i odabirom reprezentativnih uzoraka, a zavraavaju izradom PVT (engl. pressure-volume-temperature) studije koja sadr~i rezultate ispitivanja, prora una i interpretacije izvraenih eksperimenata. U proalosti su podaci iz PVT studija izravno koriateni u svrhu procjene rezervi i koli ine pridobivog fluida. Danas PVT studije predstavljaju set podataka potrebnih za prilagodbu termodinami kog modela. Na temelju termodinami kog modela, jednad~bom stanja se nadalje mogu simulirati tla no-volumno-temperaturni odnosi te promjene sastava i svojstava tekue i plinske faze za uvjete koji nisu tehni ki izvedivi u laboratoriju. Takoer, mogu se simulirati PVT analize koje nisu izvedene iz vremenskih ili financijskih razloga. Ovakve simulacije su osobito bitne kada u le~iatu, proizvodnom nizu ili u povrainskom sustavu dolazi do dvofaznog protoka. U uvjetima protoka, tj. proizvodnje iz le~iata ili utiskivanja fluida u le~iate od dijela le~iata kojeg nije zahvatila promjena tlaka u buaotinama pa do povrainskog sustava postoji visok tla ni gradijent, te neato manje izra~ene promjene u temperaturi fluida. U dvofaznom podru ju, za svaku promjenu tlaka, potrebna je analiza volumnih odnosa, viskoznosti te sastava plinske i tekue faze. Numeri ki PVT model pojedinog le~ianog fluida ulazni je podatak za in~enjerske prora une poput: prora una po etnih zaliha ugljikovodika, prora una koeficijenta iscrpka le~ianih fluida, simulacije proizvodnje iz le~iata, definiranja povezanih hidrodinami kih cjelina, interpretacije podataka o ispitivanju buaotine, usklaivanja proizvodnih podataka iz proalosti za bolju definiciju le~ianog simulacijskog modela, prora una i simulacije utiskivanja fluida u svrhu pridobivanja sekundarnim (zavodnjavanje) i tercijarnim metodama (utiskivanje plinova, otapala i sl.) te prora un optimalnih uvjeta separacije na povrainskim i procesnim postrojenjima. Laboratorijska aparatura ne mo~e mjeriti volumne promjene fluida pri temperaturi veoj od 200C. Ovo tehni ko ograni enje vodi do prve hipoteze rada: Fazno ponaaanje i volumne promjene le~ianih fluida mogue je opisati kubnom jednad~bom stanja usklaenom na PVT podatke dobivene laboratorijskim ispitivanjima pri temperaturama razli itim (manjim) od le~iane. Odreeno naftno, plinsko ili plinsko-kondenzatno polje predstavlja lokaciju na kojoj su dokazane rezerve ugljikovodika. Naj eae su ugljikovodici koji su prisutni u jednom polju nastali u jednom geoloakom periodu i sli nim uvjetima. Posljedi no mnogim geoloakim dogaanjima uslijed nastanka stijene kolektora ugljikovodika, jedno polje mo~e sadr~avati viae hidrodinami ki odvojenih jedinica (zasebnih  rezervoara ugljikovodika), tj. le~iata. Dakle, esto su ugljikovodici unutar jednog polja, a iz razli itih le~iata nastajali u sli nim uvjetima i u istom geoloakom razdoblju. Posljedica su sli ne fizikalne promjene promjenom uvjeta tlaka i temperature i stanovite razlike u sastavima na pojedinim lokacijama (dubinama). Razlike u sastavima este su i unutar jednog le~iata (jedne hidrodinami ki izolirane jedinice). Uvrije~en je naziv gradijent sastava, koji je nastao iz teoretskih razmatranja da mora postojati kontinuirana promjena u udjelima pojedinih komponenata ugljikovodika, ovisno o dubini (Riemens et al, 1988.; Montel et al., 2002; Singh et al., 2005). Kako le~iata nisu homogena, ponajviae zbog kapilarnih sila, gradijent sastava zapravo nije lako korelirati s prostornim polo~ajem uzimanja uzoraka (koordinatama i dubinama buaotina). Tako je pojam gradijent sastava zapravo sinonim za razli itosti u sastavima uzoraka uzetih iz jednog le~iata, tj. ne radi se isklju ivo o kontinuiranim promjenama udjela pojedinih komponenata u sastavu koje bi se mogle opisati gradijentom. Metode prora una i numeri ke simulacije le~iata u svrhu projektiranja dalje razrade le~iata i predikcije proizvodnje prema razli itim scenarijima iskoriatavanja (razli iti zadani tlakovi proizvodnje, utiskivanja, razmjeataja buaotina itd.) uklju uju PVT podatke o fluidima uzete na nekoliko buaotina. Postavlja se pitanje koje eksperimentalne podatke i koji PVT model uzeti kao reprezentativan za cijelo le~iate, jer u momentu kad se kree u spomenute prora une za projektiranje razrade, za svojstva fluida su dostupne PVT studije pojedina nih uzoraka fluida iz nekoliko buaotina. Stoga su koriatena provedena laboratorijska PVT ispitivanja na nizu izotermi za fluide iz razli itih tipova le~iata, od kojih svako ima izra~en gradijent sastava, s ciljem pronala~enja jedinstvene jednad~be stanja koja vrijedi za cijelo le~iate, tj. za sve fluide na odreenom podru ju koji pripadaju istom razdoblju nastanka u svrhu provjere druge hipoteze rada: kubna jednad~ba stanja definirana usklaivanjem parametara na analize uzoraka iz viae buaotina bolje e opisivati fluid u cijelom le~iatu nego ato ga opisuje jednad~ba stanja izraena na temelju reprezentativnog uzorka iz jedne buaotine. Postupak istra~ivanja Postupak istra~ivanja sa svrhom potvrde postavljenih hipoteza sastoji se od: Provedbe laboratorijskih PVT ispitivanja na viae uzoraka razli itih tipova ugljikovodika, tj. iz razli itih tipova le~iata (naftnih, plinsko-kondenzatnih) pri le~ianim temperaturama. Izrade jedinstvenih jednad~bi stanja podeaavanjem parametara razmatranih kubnih jednad~bi. Provedbe laboratorijskih PVT ispitivanja na viae uzoraka iz razli itih buaotina (pojedinog le~iata) pri temperaturama razli itim od le~iane temperature. Izrade jedinstvene jednad~be stanja kojom se najbolje mogu simulirati laboratorijski odreene analize, bez obzira na sastav. Time se dokazuje pouzdanost u simulaciji odreenih uvjeta pri kojima se mo~e nai fluid ato zna i da se istom pouzdanoau mo~e simulirati i analize koje nisu provedene u laboratoriju. Statisti ka provjera kvalitete i primjenjivosti podeaenih jednad~bi stanja  novih jednad~bi stanja pri le~ianim temperaturama, usporedbom sa pouzdanim mjerenim podacima pri le~ianoj temperaturi. Definiranje procedure PVT karakterizacije le~ianih fluida pri visokim temperaturama ili le~ianim temperaturama blizu kriti ne to ke. Pregled dosadaanjih istra~ivanja Za predikciju volumnih promjena i faznog ponaaanja le~ianih fluida (ugljikovodika) naj eae se koristi kubna jednad~ba stanja. Alternativno, za potrebe procjena pri projektiranju razrade le~iata, termodinami ka svojstva le~ianih fluida za raspon tlakova i temperatura mogue je prikazati tabli no (samo za uvjete pri kojima su mjerena te koriatenjem poopenih publiciranih korelacija za ostale uvjete, ato je nepouzdano zbog posebnosti sastava svakog le~ianog fluida), no ta metoda primjenjiva je samo za slu aj u kojemu na procjene protjecanja fluida u le~iatu bitno ne utje u fazne promjene. ak i tada preporu eno je ta svojstva potvrditi jednad~bom stanja (Whitson et al., 1988; Fevang et al., 2000; Izgec & Barrufet, 2005). Kubna jednad~ba stanja je za slo~ene smjese (poput nafte) najpogodnija zbog svoje prilagodljivosti, za razliku od viaeparametarskih jednad~bi stanja koje bi preciznije opisivale jednostavne fluide (jednokomponentne fluide ili binarne smjese). Primjenjivost i ograni enja kubnih jednad~bi stanja obrazlo~eni su u nizu radova: Martin (1967, 1979), Abbott (1979), Gray (1979), Yarbourough (1979), Tsonopolous & Heidman (1985), Firoozabadi (1988), Sreide (1989), Ashour et al. (2011) itd. U naftnoj industriji dvije su jednad~be stanja prihvaene u najairoj primjeni: Soaveova modifikacija Redlich-Kwongove jednad~be stanja (Soave, 1972) i Peng-Robinsonova jednad~ba stanja (Peng & Robinson, 1976). Egzaktnu proceduru karakterizacije le~ianih fluida jedinstvenom jednad~bom stanja dobivenom usklaivanjem njenih parametara prema izmjerenim PVT podacima viae uzoraka iz jednog le~iata predlo~ili su Whitson et al. 1989. godine. Whitsonova metoda razdjeljivanja C7+ frakcije temelji se na modelu gama distribucije i modifikaciji standardnog Gaussovog kvadraturnog pravila. Metodu je detaljno opisao i matemati ki obradio Sreide u svojoj disertaciji (1989). Valjanost metode usklaivanja parametara jednad~be stanja pomou viae uzoraka intenzivno je razmatrana posljednjih 20-tak godina (Almehaideb et al., 2000; Martinsen et al. 2010; Singh et al., 2011). Tradicionalna procedura koja se sastoji od izbora uzorka le~ianog fluida iz jedne buaotine te definicije jednad~be stanja na osnovu PVT podataka navedenog fluida i dalje je dominantno prisutna u suvremenom le~ianom in~enjerstvu (Schebetov et al., 2010; Ashour et al., 2011) svjetskih naftnih kompanija, uklju ujui i INA-e. Komponentni sastav le~ianog fluida prvi je i temeljni ulazni podatak neophodan za definiciju jednad~be stanja za taj fluid. Dio rutinske PVT-analize je i analiza komponentnog sastava le~ianog fluida kojom se odreuju molni udjeli komponenata ugljikovodika te neugljikovodi nih primjesa (sumporovodika, ugljik-dioksida, kisika, duaika). Le~iani fluidi sastoje se od dobro definiranih lakaih komponenata (C1, C2, C3, i-C4, n-C4, i-C5, n-C5, C6) i od C7+ frakcija koje se laboratorijski definiraju kao jedna pseudokomponenta. Potpuno odreivanje sastava svih komponenata u le~ianim ugljikovodicima je teako iz tehni kih razloga (sve je te~e razlikovati te~e ugljikovodike) to jest zbog injenice da C7+ frakcija sadr~i viae stotina te~ih ugljikovodi nih komponenti kao ato su parafini, nafteni, aromati, a ponekad u naftnim fluidima i asfalteni. Zbog va~nosti to no definiranog sastava, a s druge strane poznatim analiti kim metodama (plinska kromatografija, plinska kromatografija - masena spektrometrija) tehni ke nemogunosti odreivanja komponentnog sastava  plus frakcije, metode karakterizacije C7+ frakcije tema su rasprave velikog broja stru njaka (Whitson, 1983; Cotterman & Prausnitz, 1985; Whitson et al., 1989; Barrufet, 1998; Moradi et al., 2011). Martinsen et al. (2010) postavljaju normu za odreivanje faznog ponaaanja kompleksnih le~ianih fluida. Opisujui le~iate ugljikovodika s izra~enim gradijentom sastava jedinstvenom jednad~bom stanja, omoguili su to no predvianje faznog ponaaanja za procese proizvodnje i utiskivanja plina u le~iate te pouzdaniju procjenu po etnih geoloakih rezervi kondenzata/nafte i plina (Martinsen et al., 2010). U svom radu detaljno su obradili i opravdanost ulaganja dodatnih financijskih sredstava (za dodatna uzorkovanja i kompleksne PVT analize i modeliranje). Niz kompleksnih problema vezanih uz opis faznog ponaaanja le~ianih fluida rijeaeno je uz zadovoljavajuu to nost (Martinsen et al. 2010; Singh et al., 2011). Takoer su evidentna dva podru ja za koja ne postoje provjerene metode PVT karakterizacije i numeri kog odreivanja jednad~be stanja: odreivanje faznog ponaaanja fluida pri uvjetima visokog tlaka i temperature (HPHT uvjeti). laboratorijska PVT karakterizacija le~ianih fluida blizu kriti ne to ke (Luo & Barrufet, 2004). TEORIJSKO RAZMATRANJE Fazno ponaaanje le~ianih fluida nafte i plina ovisi o kemijskom sastavu. Le~iani fluidi su viaekomponentne smjese koje sadr~e primarno ugljikovodi ne spojeve od kojih veina pripada skupini alkana, te nekoliko naj eaih neugljikovodi nih spojeva (CO2, H2O, N2, H2S, O2). Uz slo~enost sastava promatrane smjese, odreivanje faznog ponaaanja le~ianih fluida ote~ava i airok raspon tla no temperaturnih uvjeta koje je potrebno obuhvatiti. Definiranje osnovnih pojmova i veli ina koji se koriste u opisu faznog ponaaanja le~ianih fluida Sastav ugljikovodi nih le~ianih fluida Broj ugljikovodi nih komponenti u prirodnoj smjesi mo~e varirati od desetak, ili manje u prirodnom plinu pa do nekoliko tisua u nafti. Potrebe za detaljnijim poznavanjem sastava nafte i kemijske prirode njenih ugljikovodi nih konstituenata puno su vee pri preradi nafte (rafinerijski procesi) nego prilikom istra~ivanja i razrade le~iata. S druge strane, volumetrijska svojstva (odnosi volumena plinske i tekue faze te gustoe faza) i transportna svojstva (viskoznosti faza, meupovrainske napetosti, mo ivost sa stijenom) od velikog su zna aja u le~ianom in~enjerstvu za velik raspon tlakova i temperatura. Spomenuta volumetrijska i transportna svojstva se bolje mogu matemati ki modelirati uz analizu sastava le~ianih ugljikovodi nih fluida koja se sastoji u kvalitativnoj i kvantitativnoj pojedina noj identifikaciji samo najlakaih ugljikovodika (od metana do pentana) dok se sadr~aj ugljikovodika vee molarne mase, odnosno, veeg broja atoma ugljika u molekuli odreuje i izra~ava udjelima pseudokomponenti, u kojima su grupirani svi ugljikovodici istog broja C-atoma, na pr. C6, C7, itd. Najstariji i analiti ki najjednostavniji na in izra~avanja sastava uklju uje grupiranje svih konstituenata, molarne mase vee od one heksana (C6) u C7+ frakciju. Plus znak uz broj C-atoma zna i da, u ovom slu aju, uz n-heptan i sve njegove izomere, plus komponenta sadr~i/uklju uje i sve ugljikovodike molarne mase vee od MC7+ bez obzira na njihov broj (koji je ionako rijetko poznat). U tablici 2-1 dan je prikaz karakteristi nih sastava le~ianih fluida. Ve prema podacima prikazanim u tablici 2-1 mo~e se zaklju iti kako komponentni sastav poma~e pri odreivanju tipa le~iata, iako je potrebno naglasiti kako sama analiza sastava ugljikovodi nih fluida nije dostatna za kona ni opis ponaaanja fluida u le~iatu. Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 1. Tipi ni sastavi i svojstva razli itih tipova le~ianih fluida (Whitson & Brul, 2000) Komponenta/ svojstvoJedinicaSuhi plinMokri plinPlinski kondenzatHlapiva naftaNaftaCO2mol%0,101,412,370,930,02N2mol%2,070,250,310,210,34C1mol%86,1292,4673,1958,7734,62C2mol%5,913,187,807,574,11C3mol%3,581,013,554,091,01i-C4mol%1,720,280,710,910,76n-C4mol%0,241,452,090,49i-C5mol%0,500,130,640,770,43n-C5mol%0,080,681,150,21C6mol%0,141,091,751,61C7+mol%0,828,2121,7656,40MC7+kg/kmol130184228274gC7+0,7630,8160,8580,920GORSm3/Sm3"18,70097026553go0,7510,7840,8350,910 Prema Whitsonu (Whitson & Brul, 2000), klju na PVT svojstva le~ianih fluida koja je potrebno odrediti kako bi bila izvediva kvalitetna potpuna karakterizacija iz koje je posljedi no mogue simulirati fluid u novim p-T uvjetima su sljedea: sastav originalnog le~ianog fluida tlak zasienja pri le~ianoj temperaturi gustoa nafte/kondenzata i plina viskoznost nafte/kondenzata i plina topivost plina u le~ianoj nafti/kondenzatu kondenzatnost le~ianog plina volumni faktori nafte/kondenzata i plina sastav ravnote~nih faza. Od nabrojanih parametara oni podcrtani izravno ovise o to nosti odreivanja sastava ugljikovodi nih smjesa te interpretaciji rezultata analiza ato ukazuje na va~nost korektne provedbe analize i interpretacije njezinih rezultata. Fazni dijagram U industriji nafte i plina od osobite va~nosti je termodinami ki opisati podru ja gdje istovremeno egzistiraju plinska i tekua faza. Jedan od najzornijih prikaza faznog ponaaanja je tla no-temperaturni (p-T) dijagram, odnosno fazni dijagram. Fazni dijagram prikazuje krivulje tlakova rosiata i zasienja koje predstavljaju granicu dvofaznog i jednofaznog podru ja. Unutar dvofaznog podru ja, naj eae se izo-linijama prikazuju udjeli ukupne tekue i plinske faze (naj eae izra~eno u volumnim ili molnim postocima tekue faze). p-T dijagram poma~e pri vizualizaciji granica jednofaznog podru ja, te promjena udjela tekue i plinske faze u dvofaznom podru ju u rasponu promjena temperature i tlaka prilikom proizvodnje fluida od le~iata do povraine, tj. sabirnog i transportnog postrojenja i koristi se pri odabiru optimalnih uvjeta proizvodnje i strategije iskoriatavanja le~iata. Na temelju polo~aja fazne krivulje i kriti ne to ke u odnosu na po etni le~iani tlak i temperaturu, le~iani fluidi u naftnom in~enjerstvu podijeljeni su u sljedeih pet kategorija: suhi plin (slika 2-1) mokri plin (slika 2-2) plinski-kondenzat (slika 2-3) hlapiva nafta (slika 2-4) nafta (slika 2-5).  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 1. Fazni dijagram suhog plina. Izotermna ekspanzija koja je mogua u le~iatu opisana je linijom od to ke 1 do to ke 2. Svi volumeni se naj eae predstavljaju relativnim omjerom volumena pri nekim le~ianim uvjetima i volumena pri separatorskim uvjetima (to ka 3). Raspon promjena temperatura i tlakova od le~iata do separatora naj eae je unutar podru ja koje bi opisale to ke 1, 2 i 3. Fluid u nijednom proizvodnom uvjetu ne dolazi u dvofazno podru je.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 2. Fazni dijagram mokrog plina. Plin u le~iatu naj eae ne dolazi u dvofazno podru je, meutim u separatorskim uvjetima dolazi do kondenzacije tekue faze.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 3. Fazni dijagram plinskog kondenzata. Plin u le~ianim uvjetima, proizvodnjom i smanjenjem le~ianog tlaka dolazi u dvofazno podru je. Dakle mogua je pojava retrogradne kondenzacije u le~iatu, tj. poveanje udjela tekue faze, a zatim opet smanjenje udjela.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 4. Fazni dijagram hlapive nafte  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 5. Fazni dijagram nafte Laboratorijska termodinami ka karakterizacija le~ianih fluida Laboratorijsko ispitivanje ugljikovodi nih fluida pri le~ianim uvjetima (PVT analiza) je eksperimentalni postupak, kojim se odreuju volumetrijske i fazne promjene le~ianog fluida. Dijagram tijeka na slici 2-6 prikazuje tijek karakterizacije naftnih le~ianih fluida, dok dijagram tijeka na slici 2-7 prikazuje tijek karakterizacije plinsko kondenzatnih le~ianih fluida.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 6. Dijagram tijeka laboratorijskog ispitivanja naftnih le~ianih fluida  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 7. Dijagram tijeka laboratorijskog ispitivanja plinsko kondenzatnih le~ianih fluida Uzorkovanje Prikupljanje pouzdanih PVT svojstava le~ianih fluida zapo inje uzorkovanjem prikladne koli ine reprezentativnog fluida na kojem se potom vrae PVT ispitivanja. Osnovni podaci zbog kojih se vrai uzorkovanje su: PVT podaci potrebni za razvoj le~ianog modela protoka (simulaciju proizvodnje, utiskivanja fluida radi poboljaanja proizvodnje, dobivanja dodatnog iscrpka ili skladiatenja, kemijske ili termalne stimulacije le~iata itd.), komponentni sastavi fluida, kvantitativna analiza ugljikovodika radi odreivanja njenih opih destilacijskih karakteristika (destilacijska krivulja odnosno volumni udjeli destilata u ovisnosti o temperaturi, cetanski broj, oktanski broj i dr.). Postupak uzorkovanja PVT uzoraka proveden je prema Radnoj uputi za dubinsko i separatorsko uzorkovanje nafte, kondenzata i plina (INA, 2003) koja je u skladu s meunarodnom normom API RP-44 (1966). Uzorkovanje mo~e biti dubinsko (slika 2-8), separatorsko i/ili povrainsko (slika 2-9), a ovisi o tipu le~iata, proizvodnim karakteristikama le~iata, stanju i opremljenosti buaotine, te konstrukciji i opremljenosti povrainskih ureaja za proizvodnju.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 8. Uzorkovanje separatorskog plina i nafte (INA, 2003)  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 9. Uzorkovanje dubinskog uzorka le~ianog fluida (INA, 2003) Izbor metode uzorkovanja ovisi o tipu le~ianog fluida koji se uzorkuje, karakteristikama proizvodnog re~ima, raspolo~ivoj opremi za provedbu uzorkovanja na terenu, te mjestu uzorkovanja. Separatorski uzorci prikladniji su za karakterizaciju plinskih te plinsko-kondenzatnih le~iata. Dubinski uzorci nafte mogu se koristiti za naftna le~iata, ukoliko su dokazano pouzdani, iako su separatorski uzorci znatno prihvatljiviji (Reudelhuber, 1954, API RP-44, 1966, McCain & Alexander, 1992, Fevang & Whitson, 1994, Gori nik, 2003). Prije uzorkovanja, bez obzira da li se radi o dubinskom ili separatorskom uzorkovanju, buaotina mora biti kondicionirana tj. u pribuaotinskoj zoni se moraju ustaliti uvjeti protoka fluida sli ni kao i u  netaknutom podru ju protjecanja, ato podrazumijeva prestanak dotoka fluida koriatenih za buaenje (isplaka i sl.) te konstantan protok tekue i plinske faze (po~eljno je da se uzorkuje u razdoblju dok tlak nije sni~en do tlaka rosiata/zasienja, tj da je u pribuaotinskoj zoni ostvaren jednofazni protok). Pad tlaka originalnog le~ianog fluida ispod tlaka zasienja mo~e rezultirati zna ajnim promjenama sastava i svojstava fluida. To ima najvei u inak na fluid oko kanala buaotine gdje je najvei pad tlaka. Cilj pripremanja buaotine za uzorkovanje (kondicioniranja) je zamjena nereprezentativnog fluida koji se nalazi u blizini kanala buaotine, originalnim fluidom iz udaljenijih dijelova buaotine. Jednostavno gaaenje proizvodnje buaotine koje za posljedicu ima obnavljanje poveanog tlaka oko buaotine nee nu~no vratiti fluidu u zahvaenom podru ju njegovo originalno stanje ili sastav. Zato je nu~no pustiti buaotinu u proizvodnju pri malim brzinama protoka kako bi originalni fluid istisnuo promijenjeni fluid. esto je potreban du~i vremenski period za kondicioniranje buaotine ato mo~e biti neprakti no s operativnog odnosno financijskog stajaliata. Kako bi se utvrdilo da li su uzorci reprezentativni, trebalo bi razmotriti prijaanja uzorkovanja i zna ajne le~iane podatke (tlak u le~iatu, tlak zasienja, plinski faktor i sl.). Kvalitetni podaci o testiranju buaotine su od neprocjenjive va~nosti za utvrivanje kvalitete uzetog uzorka le~ianog fluida. Utvrivanje da li je buaotina adekvatno pripremljena za uzorkovanje zahtijeva pa~ljivu interpretaciju trendova: tlakova na buaotinskoj glavi i dnu buaotine, brzina protoka plina odnosno nafte, proizvodnog plinskog faktora. Naravno da je za uzimanje uzoraka i dobivanje to nih mjerenja potrebna adekvatna i umjerena oprema. Pravilno pripremanje buaotine podrazumijeva proizvodnju buaotine u serijama sukcesivno ni~ih brzina protjecanja: Ukoliko je buaotina proizvodila pri njezinoj normalnoj brzini protjecanja barem 24 sata, pripremanje po inje to nim mjerenjem brzina protjecanja plina i nafte te mjerenjem tlaka protjecanja na dnu buaotine. Ukoliko su brzine plina i nafte stabilne, brzina protjecanja se smanji 30% do 50% te se periodi ki mjeri proizvodni plinski faktor sve dok se on ne stabilizira. Ova procedura smanjivanja brzine protjecanja i mjerenja plinskog faktora se ponavlja dok se ne ustanovi trend plinskog faktora s brzinom protjecanja. Iskustvo je pokazalo da prilikom smanjivanja brzine protjecanja plinski faktor mo~e ostati konstantan, smanjiti se ili poveati. Interpretacija svakog od ovih trendova nam mo~e biti smjernica za pripremanje buaotine (API RP-44, 1966). Ako plinski faktor ostane konstantan nakon prvog smanjivanja brzine proizvodnje, znat emo da nam da u kanal buaotine utje e podzasiena nafta. To zna i da su fazno stanje i sastav le~iane nafte nepromijenjeni prilikom pritjecanja nafte iz formacije u kanal buaotine. U tom slu aju smatramo da je buaotina spremna za uzorkovanje. Kao provjeru mo~emo procijeniti tlak isparavanja le~iane nafte iz proizvodnih podataka i primjenom prikladnih in~enjerskih korelacija kako bi bili sigurni da je procijenjeni tlak zasienja manji od tlaka na dnu buaotine. Smanjenje plinskog faktora nakon smanjenja brzine protjecanja nam ukazuje na prisutnost slobodnog plina u formaciji oko kanala buaotine. Zasienje formacije slobodnim plinom mo~e nastati zbog: konusiranja plinske kape u naftonosni dio formacije oko kanala buaotine, manjeg tlaka protjecanja na dnu buaotine od tlaka zasienja le~iane nafte. U tom slu aju buaotina se priprema za uzorkovanje tako da se nastavi s postepenim smanjivanjem brzine protjecanja. Nakon svake redukcije brzine, nastavlja se s protokom dok se plinski faktor ne stabilizira. Ovo stupnjevito smanjivanje brzine protoka nastavlja se sve dok se ne dobije stabilizirani (minimalni) plinski faktor. Nakon to dodatna smanjivanja brzina ne utje u na plinski faktor, sav nereprezentativni fluid je proizveden i zamijenjen s reprezentativnom naftom iz udaljenijih dijelova. Postoje i odreene korelacije koje koriatene s le~ianim tlakom i temperaturom mogu dati pribli~ne vrijednosti stabiliziranog plinskog faktora. Ako je uzrok konusiranje plina, buaotina se mo~e pripremiti u relativno kratkom vremenu tako da se brzina protjecanja smanji dovoljno kako bi eliminirala konus plina ato se mo~e vidjeti na plinskom faktoru koji bi se trebao smanjivati kako se smanjuje brzina. Poveanje plinskog faktora nakon smanjivanja brzine protjecanja je indikator istovremene kombinirane proizvodnje plina iz plinonosne zone i nafte iz naftonosne zone. Poveanje plinskog faktora mo~e biti uzrokovano konusiranjem nafte. Iako se esto mo~e dobiti reprezentativan uzorak nafte, bolje je koristiti buaotine koje ne ukazuju na znakove konusiranja nafte zato ato je u tom slu aju teako odrediti kada je buaotina adekvatno pripremljena za uzorkovanje. Vrijeme potrebno za stabiliziranje plinskog faktora mo~e ovisiti viae o povla enju naftnog konusa nego o brzini protjecanja i volumenu nereprezentativne nafte koju treba protisnuti reprezentativna nafta. Kondicioniranje naftne buaotine je proces eliminiranja bilo kojeg konusiranja plina i ispiranje nafte, iji je sastav promijenjen zbog izlo~enosti tlaku manjim od tlaka zasienja, iz pribuaotinske zone. Nereprezentativna nafta se istiskuje reprezentativnom naftom iz udaljenijih dijelova le~iata sa stupnjevitim smanjivanjima brzine proizvodnje. Stabilizirani proizvodni plinski faktor se mjeri nakon svakog smanjenja brzine protjecanja. Smatra se da je buotina kondicionirana kada daljnja smanjenja brzine protoka nemaju utjecaj na proizvodni plinski faktor. Procedura za kondicioniranje plinsko kondenzatnih le~iata je temeljena na interpretaciji promjene proizvodnog plinskog faktora pri stupnjevitom smanjenju brzine proizvodnje. Kada se tlak plinsko kondenzatnog fluida smanji ispod to ke rosiata, dolazi do formiranja tekue faze odnosno kondenzata. Rezultat toga je da e plinovita faza, koja je dominantna u proizvodnom fluidu imati ni~u koncentraciju od tekuih ugljikovodika (posebno te~ih ugljikovodika). Ovaj gubitak tekuih ugljikovodika obi no u po etku rezultira poveanim proizvodnim plinskim faktorom. Budui da se najni~i le~iani tlak javlja u pribuaotinskom podru ju, retrogardni fluid (kondenzat) e prvo kondenzirati u podru ju oko buaotine. U daljnjem nastavku proizvodnje, zasienje kondenzatnom tekuinom u tom podru ju mo~e narasti dovoljno (ali ne u svim slu ajevima) da tekuina postane mobilna. Poveanje ove mobilne tekuine mo~e smanjiti proizvodnost buaotine i uzrokovati nepredvidive, ali zna ajne kratkoro ne promjene proizvodnog plinskog faktora zbog promjena u brzinama proizvodnje. Prema API RP-44 (1966), cilj uzorkovanja le~ianog fluida je sakupiti uzorak koji vjerno predstavlja fluid prisutan u le~iatu u vrijeme uzorkovanja, odnosno identi an sastavu fluida u le~iatu. Ukoliko se uzorkuje na pogreaan na in ili nije bilo ispravnog kondicioniranja buaotine, mogue je da uzorci ne budu reprezentativni. U RP-44 takoer stoji kako uporaba podataka dobivenih ispitivanjima nereprezentativnog fluida, bez obzira na kvalitetu provedbe laboratorijskih ispitivanja, rezultira pogreanim upravljanjem le~iata. Uzorkovanje je prvi put potrebno izvraiti kada je tlak le~iata joa uvijek iznad tlaka zasienja jer je tada fluid joa jednofazan, tj. dovoljno rano u proizvodnji le~iata. Uzorkovanje se mo~e ponoviti nakon nekog perioda proizvodnje, zbog promjena tlaka u le~iatu (zbog horizontalnog gradijenta tlaka od buaotine do tla nom depresijom netaknutih dijelova le~iata) i zaostajanja te~ih ugljikovodika u podru jima udaljenijim od buaotina (pokretljivost te~ih ugljikovodika je manja od lakaih, tj. manja je relativna propusnost). Veina stru njaka tvrdi da nakon ato le~iani tlak padne ispod tlaka zasienja, viae nije mogue dobiti uzorak originalnog le~ianog fluida (API, 1966, Gori nik, 2003; Nagarajan et al., 2006). Naime, kada tlak u pri-buaotinskoj zoni padne ispod tlaka zasienja originalnog le~ianog fluida, odvajaju se dvije faze (plinska i tekua) razli itog sastava. To gotovo uvijek rezultira razli itim protokom plinske i tekue faze u kanalu buaotine te uslijed toga dolazi do razli itog sastava proizvodnog fluida od sastava po etnog, originalnog le~ianog fluida. Nasuprot veine, Fevang & Whitson (1994, 1998) tvrde kako je svaki fluid proizveden iz le~iata reprezentativan za to le~iate jer on to upravo i je  uzorak proizveden iz tog le~iata. Kona na jednad~ba stanja le~ianog fluida treba moi matemati ki simulirati sve to no izmjerene PVT podatke svih uzoraka proizvedenih iz le~iata, neovisno o tome da li je neki uzorak reprezenatativan  originalni le~iani fluid. `toviae, jednad~bom stanja se predviaju promjene u sastavu fluida tijekom crpljenja le~iata ato predstavlja puno veu razliku u sastavu od razlike izmeu reprezentativnog ili nereprezentativnog uzorka. Obrada nereprezentativnih uzoraka, u svrhu dobivanja kvalitetnih podataka o sastavu i PVT svojstvima, prema Fevang & Whitson (1994) ispitana je u INA-inom laboratoriju i prezentirana na 4. Meunarodnom znanstveno-stru nom skupu o naftnom gospodarstvu (Belamari et al., 2009). Kontrola kvalitete uzoraka Kontrola kvalitete uzoraka provodi se prije po etka analize s ciljem utvrivanja tlaka i faznog stanja fluida u spremnicima s uzorcima Kontrola tlaka vrai se umjerenim manometrom. Usporeuju se tlak uzorkovanja i tlak u boci za uzorkovanje. Tolerira se razlika u tlakovima do 10% od tlaka uzorkovanja, do koje mo~e doi uslijed razlike u temperaturi. Kontrola faznog stanja tekueg uzorka vrai se viaekratnim injektiranjem unaprijed odreenog volumena ~ive u bocu s uzorkom. Ukoliko se tlak uzorka brzo stabilizira te ako su volumeni injektirane ~ive po jedinici tlaka jednaki, uzorak je jednofazan i ispravan. Na temelju rezultata kontrole uzoraka te vrsti uzoraka odreuje se daljnji tijek analiza. PVT testovi Analiza sastava i svojstava plina i nafte/kondenzata Sastavi plinske i tekue faze ugljikovodi nih fluida odreuju se metodom plinske kromatografije. Plinska kromatografija je fizikalna metoda odjeljivanja u sustavu stacionarne faze (kruta tvar vrlo velike specifi ne povraine ili kruti nosa  natopljen tekuinom) smjeatene u kromatografskoj koloni i mobilne faze (plinovi: helij, duaik ili vodik). Ispitivani uzorak (smjesa tvari) uvodi se pomou struje inertnog plina nosioca u kromatografsku kolonu ispunjenu krutom ili tekuom stacionarnom fazom. Odreivanje duaika, uglji nog dioksida i ugljikovodika od C1 do C14 u plinu izvodi se koriatenjem etiri-kolonskog sustava spojenog s tri ventila za provedbu injektiranja i ulaza uzorka u kanal s kapilarnom kolonom i plameno ionizacijskim detektorom (engl. Flame Ionisation Detector  FID) ili kanal s pakiranim kolonama i detektorom toplinske vodljivosti (engl. Thermal Conductivity Detector  TCD), gdje prisutnost komponenata u plinu nosiocu izaziva odgovarajui signal na detektoru, ija je povraina proporcionalna koncentraciji komponente u plinu nosiocu. Signal se prenosi na pisa  kao otklon od osnovne linije u funkciji s vremenom u formi Gaussove krivulje (slika 2-10).  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 10. Kromatogram uzorka prirodnog plina Analize tekuih ugljikovodi nih fluida analiziraju se u skladu s metodom ASTM  Standard D 2887 (2008). Frakcije nafte dobivene destilacijom ili otplinjeni uzorci separatorskog kondenzata pohranjeni su u staklene posude s bruaenim epom pri atmosferskom tlaku. Uzorak mora biti homogen. Eventualno istalo~ene parafine treba otopiti blagim zagrijavanjem. Prije samog mjerenja, potrebno je analizirati kvalitativne certificirane test smjese kako bi se identificirale prisutne komponente i pratilo razdvajanje na koloni. Rezultat analize predstavlja kromatogram (slika 2-11) iz kojeg se ra unaju povraine ispod zabilje~enih otklona na kromatogramu integracijom krivulje u podru ju otklona. Izvjeataj nakon zavraene analize sastoji se od kromatograma, kvalitativne i kvantitativne analize s podacima (vrijeme zadr~avanja, povraina, maseni udio komponente).  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 11. Analiza nafte na plinskom kromatografu Agilent Technologies 6890N Identifikacija komponenata i otklona ( pikova ) na kromatogramu n-parafina C2-C50 vrai se usporedbom sa poznatim vremenom zadr~avanja (engl. Retention Time, RT) ovih komponenata iz analize jedne ili viae test smjesa. i-parafini (istog broja ugljikovih atoma) eluiraju prije pripadnog n-parafina. U posebnim slu ajevima na isti na in se vrai identifikacija aromata. Povraine ispod pikova grupiraju se po odreenim intervalima prema vremenu zadr~avanja i dobiju se podaci o masenim udjelima parafina u uzorku. Kvantitativna analiza podrazumijeva normalizaciju povraina pikova i grupiranje masenih postotaka izo i n-parafina. Navedeni rezultati koriste se kao ulazni podaci za prora un sastava plinsko-naftnih le~ianih fluida ili za prora un sastava plinsko-kondenzatnih fluida iz protoka buaotina. Kontaktno otplinjavanje (flash) separatorske nafte/kondenzata Kontaktno otplinjavanje separatorske tekue faze prvi je korak, nakon provjere kvalitete uzoraka, u laboratorijskoj karakterizaciji ugljikovodi nih fluida. Mjerenjem volumnih i faznih promjena fluida pri separatorskoj temperaturi, te jednostupanjskom separacijom do standardnih p-T uvjeta odreuju se slijedei podaci o separatorskom kondenzatu: plinski faktor, volumni faktor separatorske tekue faze, koeficijent stla ivosti fluida, koeficijent termi ke ekspanzije. Plinski faktor (GOR) definiran je kao omjer volumena plina uobi ajeno izra~en u metrima kubnim pri standardnim uvjetima po volumenu nafte izra~enim u metrima kubnim pri separatorskim uvjetima. Volumni faktor (B) karakterizira volumetrijsko ponaaanje odreenog fluida (nafte, plina ili slojne vode) pri promjeni tlaka i temperature te je definiran kao omjer volumena fluida pri nekim uvjetima tlaka i temperature (le~ianim, buaotinskim, separatorskim) i volumena istog tog fluida pri standardnim uvjetima (Gori nik, 2006). Volumni faktor se obi no ra una na temelju laboratorijskih analiza koje su raene za le~ianu izotermu i njime je pojednostavljeno prera unavanje volumena doti nih fluida iz mjerenih proizvodnih uvjeta na povraini u neke druge uvjete, naj eae le~iane. Volumni faktori slojne vode i nafte, prakti ni su iz razloga jer uklju uju volumnu promjenu zbog otparavanja plina uslijed smanjenja tlaka (i iz tog razloga je vei od 1). Koeficijent stla ivosti fluida (nafte) (c) ra una se za jednofazno podru je nafte kao omjer promjene volumena nafte po promjeni tlaka pomno~en s recipro nom vrijednoau volumena nafte:  EMBED Equation.3  (bar-1) (2-1) Koeficijent termi ke ekspanzije (nafte) (b) ra una se za jednofazno podru je nafte kao omjer promjene volumena nafte po promjeni temperature pomno~en s recipro nom vrijednoau volumena nafte:  EMBED Equation.3  (C-1) (2-2) Prije daljnje upotrebe laboratorijskih podataka za podeaavanje parametara jednad~be stanja, podaci se moraju provjeriti obzirom na sastave proizvedenih fluida, K-omjere separatorskih fluida te proizvodne uvjete tijekom vremena proizvodnje. Ravnote~ni K-omjeri kvantitativno opisuju raspodjelu svake komponente "i" sustava izmeu plinske i tekue faze, tj. koncentracije komponente u fazama kod ravnote~nih p,T uvjeta:  EMBED Equation.3  (2-3) gdje su: Ki ravnote~ni omjer ("konstanta") komponente "i" yi molni udio komponente  i u plinskoj fazi xi molni udio komponente  i u tekuoj fazi Podaci dobiveni odreivanjem sastava i kontaktnim otplinjavanjem koreliraju se na sljedee na ine: grafi ki se provjerava slaganje relativne gustoe i molarne mase C7+ frakcije separatorskog kondenzata, radi se pregled promjena separatorskih uvjeta i proizvodnog plinskog faktora kroz vrijeme, grafi ki se prikazuje odnos molnog udjela na logaritamskoj skali obzirom na jedinstveni uglji ni broj (engl. Single Carbon Number, SCN) u uzorku separatorskog kondenzata na linearnoj skali za odabrane setove podataka (pribli~no ravna linija), radi se provjera K-omjera od metana do heksana pri uvjetima separacije na polju koriatenjem Hoffman-Crump-Hocott metode te usporedba linearnog trenda s vrijednostima Standingove jednad~be za odabrane setove podataka. Slaganje relativne gustoe i molarne mase C7+ frakcije separatorske kapljevine Watsonov ili UOP (engl. Universal Oil Products) karakterizacijski faktor dovodi u odnos temperaturu vreliata izra~ene u kelvinima i relativnu gustou sljedeom jednad~bom:  EMBED Equation.3  (2-3) gdje su: Kw Watsonov karakterizacijski faktor Tb temperatura vreliata (K) g relativna gustoa Watsonov karakterizacijski faktor prikazan odnosom molarne mase i relativne gustoe prema Whitsonu (1983) mogue je izraziti jednad~bom:  EMBED Equation.3  (2-4) gdje je: M molarna masa (g/mol) Kw varira od 8,5 do 13,5 ovisno o sastavu (odnosno molarnoj masi i relativnoj gustoi). Ugrubo vrijedi: za parafine Kw=12,5 do 13,5; za naftene Kw=11,0 do 12,5 te za aromate Kw=8,5 do 11,0. Austad et al. (1983) u svom radu, na osnovu statisti ke obrade podataka za polja Sjevernog mora, zaklju uju kako je Watsonov karakterizacijski faktor ra unat kao  EMBED Equation.3  i  EMBED Equation.3  esto konstantan za odreeno polje ak i tijekom proizvodnje te ak i ako relativna gustoa varira. Whitson et al. (1998) navode granice prihvatljivosti odstupanja Kw 0,03, dok Gori nik (2004) proairuje te granice na 5% odstupanja molarne mase. Proizvodni parametri Ukoliko se ne radi o novom polju, te postoje podaci o separatorskim uvjetima i proizvodnim plinskim faktorima, mogue je napraviti pregled tijekom cjelokupnog vijeka proizvodnje promatranog polja. Kako je est slu aj da se tijekom viaegodianje proizvodnje i uzorkovanja mijenjaju uvjeti separacije, esto nije mogue na osnovu tih podataka izvesti zaklju ak, ali je mogue dovesti u vezu promjenu tlaka le~iata i ukupnog proizvodnog plinskog faktora tijekom ukupnog vremena proizvodnje. O ekuje se pad le~ianog tlaka te analogno tome porast ukupnog proizvodnog plinskog faktora. Proizvodni plinski faktor definira se kao volumen separatorskog plina pri standardnim uvjetima po volumenu separatorske nafte pri separatorskim uvjetima:  EMBED Equation.3  (m3sc/m3sep) (2-5) Whitson (1998) procjenjuje pogreaku proizvodnog plinskog faktora od 5 do 15%. Mogue su i vee pogreake za lagane plinsko-kondenzatne sustave koji se proizvode u velikim koli inama. Nekoliko je moguih izvora tako velike pogreake: neto no izmjerena koli ina proizvedene nafte, neto no izmjerena koli ina proizvedenog plina, neto an faktor pretvorbe plina iz separatorskih na standardne uvjete, prijenos separatorske kapljevine u struju separatorskog plina, kombinacija svega navedenog. Sastav stabilizirane tekue faze (nafte ili kondenzata) Pedersen et al. (1989) dokazali su da je grafi ki prikazan odnos molnog udjela i molarne mase, odnosno jedinstvenog uglji nog broja, eksponencijalan za plinsko-kondenzatne sisteme. To opa~anje rezultiralo je ope prihvaenim zaklju kom da je relacija izmeu molnog udjela na logaritamskoj skali i pripadajueg jedinstvenog uglji nog broja na linearnoj skali ravna linija. Sastavi separatorskih fluida Konzistentnost sastava separatorskog plina i kapljevine mogue je provjeriti Hoffman-Crump-Hocott grafi kom metodom. Hoffman et al. (1953) dokazali su da log vrijednosti K-omjera u odnosu na faktor Fi mora rezultirati ravnom linijom. Hoffmanov faktor Fi ra una se pomou jednad~be:  EMBED Equation.3  (2-6) gdje su:  EMBED Equation.3  temperatura vreliata komponente i (C)  EMBED Equation.3  temperatura separacije (C)  EMBED Equation.3  konstanta komponente i Standing (1979) daje modificirane vrijednosti za  EMBED Equation.3  i  EMBED Equation.3  koje se od tada koriste u Hoffman et al. metodi. Prema Standingu, korelacija vrijedi do tlaka od 70 bar i za raspon temperature od 5 do 95C. Dijagram izmjerenih K-omjera koristei ovu metodu ne bi smio zna ajnije odstupati od Standingove ravne linije. Prema Whitsonu (1998)  EMBED Equation.3 -frakcija, neugljikovodi ne komponente te komponente molnog udjela manjeg od 0,5% mogu odstupati od Standingove linije. Ali ako ugljikovodi ne komponente od metana do heksana pokazuju zna ajno odstupanje od ravne linije, analiza sastava se ne smije uzeti sa sigurnoau. Rekombinacija le~ianog fluida Provodi se na temelju rezultata ispitivanja separatorskog plina i separatorske nafte/kondenzata. Fizi ka rekombinacija le~ianog fluida mo~e se provesti u eliji za rekombinaciju ili direktno u PVT eliji u kojoj e se vraiti daljnja ispitivanja, ovisno o tipu fluida i planiranim ispitivanjima. Sam postupak sastoji se u utiskivanju separatorskog plina u unaprijed odreen vakuumirani volumen PVT elije te zatim dodavanja pripadajueg volumena separatorske tekue faze koji se ra una obzirom na proizvodni plinski faktor odreen na separatoru tijekom uzorkovanja. Sva daljnja PVT ispitivanja (test ekspanzije pri stalnom sastavu, separator test, testovi otparavanja, viskoznost) vrae se na rekombiniranom le~ianom fluidu. Test ekspanzije pri stalnom sastavu Test ekspanzije pri stalnom sastavu (engl. Constant Composition Expansion, CCE) rekombiniranog le~ianog fluida provodi se pri le~ianoj temperaturi. Volumne promjene fluida tijekom ekspanzije zbog smanjivanja tlaka prate i fazne promjene fluida (retrogradna kondenzacija kod plinsko kondenzatnih sustava). Shematski prikaz procesa testa ekspanzije pri stalnom sastavu nafte dan je na slici 2-12.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 12. Shematski prikaz testa ekspanzije nafte Tlakovi zasienja le~ianog fluida vizualno se o itavaju tijekom testa ekspanzije pri stalnom sastavu. Tlak isparavanja (pb) je tlak pri kojem se pojavljuje prvi mjehuri pare, odnosno, to je tlak pri kojem je tekua faza u ravnote~i s beskona no malom koli inom plinske faze (Gori nik, 2006). Tlak rosiata (pd) je tlak pri kojem po inje kondenzacija, odnosno, to je tlak pri kojem je plinska faza u ravnote~i s beskona no malom koli inom tekue faze (Gori nik, 2006). Tlak zasienja (ps) je izraz koji se esto koristi umjesto tlaka isparavanja za naftne, odnosno tlaka rosiata za plinsko kondenzatne fluide (Gori nik, 2006). Iz mjerenih volumetrijskih podataka ra unaju se: relativni volumen fluida (iz testa izotermne ekspanzije fluida stalnog sastava), volumni faktor fluida, te volumni udio kondenzata kao funkcija tlaka i temperature. Relativni volumen fluida stalnog sastava (Vrel) funkcija je tlaka pri konstantnoj temperaturi, te je pri le~ianoj temperaturi definiran kao omjer ukupnog volumena fluida i volumena fluida pri tlaku zasienja:  EMBED Equation.3  (2-7) Volumni udio kondenzata (Vliq) mo~e se izraziti volumnim udjelom kondenzata u ukupnom volumenu fluida ili volumnim udjelom kondenzata u volumenu pri tlaku zasienja. Prvi na in rabi se pri interpretaciji rezultata retrogradne kondenzacije tekue faze tijekom testa ekspanzije pri stalnom sastavu, dok se drugi na in rabi pri usporedbi volumetrijskih podataka testa ekspanzije pri stalnom sastavu i podataka iz testa otparavanja pri stalnom volumenu (Gori nik, 2006):  EMBED Equation.3  (2-8) Diferencijalno otparavanje Diferencijalno otparavanje (engl. Differential Liberation, DL) provodi se nakon prora una testa ekspanzije pri stalnom sastavu. Rekombinirani ili dubinski uzorak le~iane nafte stabilizira se pri le~ianoj temperaturi na tlaku zasienja. Nakon stabilizacije uzorka nastavlja se sa stupnjevitim sni~avanjem tlaka (uobi ajeni koraci Dp=20 bar) do atmosferskog. Osloboeni plin pri svakom tlaku uklanja se iz elije uz podr~avanje konstantnog tlaka preostalog fluida i analizira sastav plina. Parametri koji se mjere i iskazuju za svaki pojedini stupanj su: volumni faktor nafte i faktor otopljenog plina kao funkcija tlaka, gustoa nafte pri le~ianim uvjetima, te sastav, gustoa i kompresibilnost osloboenog plina. Faktor otopljenog plina (Rs) definiran je kao omjer volumena isparenog plina na n-tom stupnju otparavanja izra~en pri standardnim uvjetima i volumena proizvedene nafte pri standardnim uvjetima. Shematski prikaz procesa testa diferencijalnog otparavanja nafte dan je na slici 2-13.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 13. Shematski prikaz testa diferencijalnog otparavanja Separator test Laboratorijskim testom separacije nafte pri razli itim p,T-uvjetima odreuju se optimalni uvjeti rada proizvodnog separatora na polju sa stanoviata relativnih proizvedenih koli ina plina i nafte. Separatorski test nafte na uzorku slojne nafte je jedno ili viae stupanjska separacija plina i nafte pri razli itim p,T uvjetima uklju ujui povrainske (standardne) p,T uvjete. Volumne promjene nafte od slojnih do standardnih uvjeta, volumen osloboenog plina, te analiti kim metodama odreeni sastav plina i gustoa fluida definiraju slijedee parametre: plinski faktor nafte i volumni faktor nafte. Na po etku testa se le~iani fluid nalazi pri uvjetima zasienja te se mjeri njegov volumen. Nakon toga se uzorak stabilizira na uvjete prvog stupnja separacije. Izdvaja se plinska faza te se bilje~e volumen nafte pri prvom stupnju separacije, volumen izdvojenog plina, koli ina tvari izdvojenog plina i relativna gustoa izdvojenog plina. Izdvojenom plinu se kromatografskom analizom odredi komponentni sastav. Nakon izdvajanja osloboene plinske faze, preostala nafta stabilizira se na uvjete sljedeeg stupnja separacije. Ponovno se izdvaja nova plinska faza te joj se odreuje komponentni sastav i relativna gustoa. Bilje~i se volumen nafte te se proces ponavlja sve dok se ne postignu standardni uvjeti. Zavrani volumen i relativna gustoa nafte mjere se pri 15C. Shematski prikaz separator testa je na slici 2-14.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 14. Shematski prikaz testa viae stupanjske separacije nafte (Whitson & Brul, 2000) Viskoznost Pri le~ianoj temperaturi viskoznost nafte mjeri se u visokotla nom viskozimetru s kotrljajuom kuglicom. Pri odreenom tlaku i temperaturi viskoznost nafte je funkcija gustoe nafte i vremena prolaza kuglice. Tijekom analize mjeri se viskoznost nafte pri le~ianoj temperaturi za tlakove od maksimalnog radnog (400 bara) do atmosferskog. Rezultati mjerenja iskazuju viskoznost kao funkciju tlaka pri le~ianoj temperaturi. Test otparavanja pri stalnom volumenu Test otparavanja pri stalnom volumenu (engl. Constant Volume Depletion, CVD) provodi se nakon testa ekspanzije pri stalnom sastavu. Uzorku kondenzatnog fluida odredi se volumen pri temperaturi le~iata i tlaku rosiata ili pri temperaturi i tlaku le~iata. Ovaj volumen je stalni volumen tijekom testa. Stupnjevito smanjenje tlaka posti~e se odgovarajuim poveanjem volumena. Svaki stupanj tla ne depresije uklju uje izobarno uklanjanje plinske faze sve dok volumen fluida ne poprimi po etnu,  stalnu vrijednost. Pri svakom tla nom koraku mjeri se: volumni udio tekue faze (kondenzat) u preostalom fluidu, volumen osloboenog plina i ukapljenog kondenzata, sastav osloboenog plina i kondenzata. Iz mjerenih podataka odreuje se za svaki tla ni korak testa: volumni faktori kao funkcija tlaka, Z faktor, te gustoe, sastavi, molarne mase i molni udjeli proizvedenog plina i kondenzata. Z faktor (sinonimi: korekcijski faktor, faktor odstupanja, faktor stla ivosti ili faktor kompresibilnosti plina) definiran je kao omjer volumena realnog plina po volumenu idealnog plina pri odreenim p, T uvjetima za specifi an sastav plina. Shematski prikaz procesa testa otparavanja plinskog kondenzata pri stalnom volumenu dan je na slici 2-15.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 15. Shematski prikaz testa otparavanja pri stalnom volumenu (Gori nik, 2006) Materijalno uravnote~enje podataka iz testa otparavanja pri stalnome volumenu Reudelhuber i Hinds (1957) razradili su metodu materijalnog uravnote~enja za test otparavanja pri stalnom volumenu. Ra un materijalnog uravnote~enja su 1983. godine dodatno razradili i objasnili Whitson i Torp. Jedan od najva~nijih podataka koje proizlaze iz testa otparavanja pri stalnom volumenu (CVD) je prora un sastava tekue faze pomou kojeg je, zajedno s kromatografski odreenim sastavom plinske faze, mogue odrediti ravnote~ne K omjere (nezaobilazan dio nekoliko va~nih razradnih i proizvodnih aplikacija). K omjer ili ravnote~ni omjer je kvocijent molnog udjela komponente i u parnoj i tekuoj fazi pri specificiranom ravnote~nom tla no temperaturnom uvjetu (Gori nik, 2006). Po etne postavke ra una materijalnog uravnote~enja su jednad~be 2-9 i 2-10.  EMBED Equation.3  (2-9)  EMBED Equation.3  (2-10) gdje su :  EMBED Equation.3  ukupan broj molova sistema na k-tom stupnju CVD-a (mol)  EMBED Equation.3  broj molova tekue faze sastava xj (mol)  EMBED Equation.3  broj molova plinske faze sastava yj (mol) indeks j ozna ava pojedinu komponentu, a k pojedini tla ni korak CVD-a. Ra un se temelji na pretpostavljenoj po etnoj koli ini tvari od 1 mol.  EMBED Equation.3  (2-11)  EMBED Equation.3  (2-12) gdje su:  EMBED Equation.3  koli ina proizvedenog fluida na i-tom koraku CVD testa (mol)  EMBED Equation.3  po etni sastav fluida u prvom koraku CVD-a (kod tlaka zasienja) Broj molova plinske faze preostale u eliji se izra una preko zakona za realne plinove (pV=ZnRT).  EMBED Equation.3  (2-13) gdje su :  EMBED Equation.3  volumen elije (m3)  EMBED Equation.3  faktor kompresibilnosti plina kod tlaka rosiata  EMBED Equation.3  plinska konstanta = 0,083143 Jmol-1K-1  EMBED Equation.3  temperatura (K)  EMBED Equation.3  tlak rosiata (bar)  EMBED Equation.3  (2-14) gdje su:  EMBED Equation.3  volumen tekue faze (cm3)  EMBED Equation.3  udio tekue faze u odnosu na ukupan volumen elije u postotku (odreen vizualno) Iz volumne bilance slijedi:  EMBED Equation.3  (2-15) gdje je:  EMBED Equation.3  volumen plinske faze Ponovo koristei zakon za realne plinove pripadajui broj molova plinske faze iznosi:  EMBED Equation.3  (2-16) Z faktor plina o itamo iz Standing-Katz-ovog dijagrama (Standing & Katz, 1942). U ovoj fazi, odreene su sve nepoznanice iz jednad~be 2-9 osim sastava tekue faze. U svrhu dobivanja sastava tekue faze prilagoena jednad~ba 2-9 sada glasi:  EMBED Equation.3  (2-17) K omjer, odnosno omjer fazne ravnote~e definiran je kao:  EMBED Equation.3  (2-18) Iz ra una masene bilance 2-19 dobivaju se potrebni podaci o fizikalnim svojstvima fluida.  EMBED Equation.3  (2-19) gdje su :  EMBED Equation.3  ukupna masa sistema (g)  EMBED Equation.3  masa tekue faze (g)  EMBED Equation.3  masa plinske faze (g)  EMBED Equation.3  (2-20) gdje su :  EMBED Equation.3  po etna molarna masa (kod tlaka rosiata) (gmol-1)  EMBED Equation.3  molarna masa plinske faze na i-tom koraku CVD testa (gmol-1) Md i Mv ra unaju se preko Kay-evog zakona mijeaanja.  EMBED Equation.3  (2-21)  EMBED Equation.3  (2-22) Izra unavai mase i volumene ravnote~ne plinske i tekue faze, odgovarajue gustoe se ra unaju direktno iz =m/V (volumeni iz jednad~bi 2-14 i 2-15. Prilagodbom jednad~be masene bilance, takoer je mogue odrediti molarnu masu tekue faze i posebno C7+ frakcije (jednad~be 2-24 i 2-25.  EMBED Equation.3  (2-23)  EMBED Equation.3  (2-24)  EMBED Equation.3  (2-25) gdje je:  EMBED Equation.3  molarna masa iste komponente (kg/kmol) Provjera K-omjera Bashbush (1981) preporu a proceduru za provjeru konzistentnosti eksperimentalnih podataka testova u pet koraka: Grafi ki prikaz komponentnog sastava proizvedenog plina (yi) na logaritamskoj skali u odnosu na tlak trebale bi biti izglaene linije.  Grbe na grafu ukazuju na eksperimentalne pogreake. Dvofazni Z faktor kod plinskih kondenzata ne bi se smio razlikovati na treoj decimali viae od jedan za sva mjerenja. Zadovoljavanje ovog uvjeta nije kona no, odnosno ne dokazuje konzistentnost eksperimentalnih podataka. Analiza sastava tekue faze pri zadnjem koraku otplinjavanja ne smije odstupati u odnosu na izra unati sastav tekue faze viae od 1% za sve komponente molnog udjela veeg od 0,4%. Grafi ki prikaz komponentnog sastava tekue faze (xi) na logaritamskoj skali u odnosu na tlak. Jednako kao u prvom koraku, linije moraju biti izglaene. Grafi ki prikaz K omjera izra unatog tijekom provedbe prora una materijalnog uravnote~enja na logaritamskoj skali u odnosu na tlak. Krivulje bi trebale biti trenda sli nog paralelnom, bez  grba i kri~anja. Slika 2-16 (Martinsen et al., 2010) prikazana je kao primjer konzistentnih PVT podataka tijekom provedbe testa ekspanzije pri konstantnom sastavu. Ovaj korak su dodali Samaniego et al. (2004). Grafi ki prikaz K omjera pojedine komponente na logaritamskoj skali u odnosu na temperaturu vreliata te komponente. Za dobro provedene PVT eksperimente ovaj graf trebao bi biti pravac.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 16. Primjer provjere K-omjera (Martinsen et al., 2010) Procjena nesigurnosti termodinami kih parametara Procjena proizvodnje/dobivanja ugljikovodika iz le~iata temelji se na podacima koji u prora un unose razli ite nivoe nesigurnosti. Utjecaj svake pojedina ne nesigurnosti potrebno je posebno istra~iti kako bi se mogao odrediti njihov ukupan utjecaj. Ukoliko se razmatra potreba za definiranje izvora nesigurnosti, nu~no je uzeti u obzir ne samo korist procjene ve i troaak ignoriranja nesigurnosti. Loae odluke mogu biti temeljene na loaoj procjeni nesigurnosti jednako kao i na loaim podacima (Trengove et al., 1991). Procjena nesigurnosti PVT podataka izuzetno je bitna jer omoguava ispravno ponderiranje eksperimentalnih rezultata koji se koriste pri podeaavanju parametara jednad~be stanja. Nije mogue postaviti openite tvrdnje o to nosti PVT podataka, budui da razli iti laboratoriji obavljaju ispitivanja na razli ite na ine i ne postoje dva identi na le~iana fluida niti njihove studije. Bansal (1988) je istra~io osjetljivost rezultata simulacije hlapive nafte na PVT podatke, posebice: plinski faktor (GOR), slojni volumni faktor (FVF, Bo), tlak zasienja (pb) i viskoznost nafte. Najvei utjecaj od promatranih parametara ima tlak zasienja. Ukoliko je tlak zasienja za 10% ni~i, simulirani proizvodni plinski faktor nakon 5 godina za buaotine koje se nalaze prema vrhu strukture manji je i za 34%, a utok vode vei je za 10%. To nost eksperimentalnih PVT podataka Eyton (1987) razmatra to nost veine eksperimentalnih podataka koriatenih i dobivenih tijekom testa ekspanzije pri konstantnom volumenu. Eyton daje sljedee mjerne nesigurnosti: omjer volumena kondenzata i plina (engl. condensate to oil ratio, CGR) tijekom CVD-a: 5-10% gustoa tekue faze  najvea to nost CGR dobiven tijekom kontaktnog otplinjavanja (flash)  najmanja to nost (jako ovisi o brzini provedbe samoga testa) loae uzorkovanje na terenu nije mogue ispraviti u laboratoriju volumeni tekue faze tijekom CVD-a sistematski su podcijenjeni  ukazuje na ovisnost volumena tekue faze o vremenu stabilizacije pri pojedinom tla nom koraku. Eyton (1987) tvrdi kako se svaki fluid stabilizira nakon dva i pol sata stabilizacije, dok veina laboratorija stabilizira fluide pola sata izmeu pojedinog tla nog koraka. Neovisno o Eytonu (1987), Drohm et al. (1988) statisti ki su obradili podatke iz 80 PVT studija. Iz baze podataka (od 80 PVT analiza) prepoznati su sljedei u estali problemi: negativan udio komponente u tekuoj fazi  EMBED Equation.3  (2-26) gustoa tekue faze vea od gustoe vode ili poveanje gustoe tekue faze porastom tlaka  EMBED Equation.3  (2-27) krivulja zasienja retrogradnim kondenzatom ima  rep  konkavan oblik kod tlaka zasienja  EMBED Equation.3  (2-28) faktor otopljenog plina pada s porastom tlaka  EMBED Equation.3  (2-29) Rezultati statisti ke obrade podataka s obzirom na navedene probleme su sljedei: negativan udio komponente u tekuoj fazi: 71 PVT analiza. Veina eksperimenata povezuje ovaj problem s lakaim komponentama. prevelika gustoa tekue faze: 45 fluida poveanje gustoe tekue faze s porastom tlaka: 66 PVT analiza za jedan ili viae tlakova krivulja zasienja retrogradnim kondenzatom ima  rep kod tlaka zasienja: 40 analiza faktor otopljenog plina pada s porastom tlaka: 53 eksperimenta. Ovaj problem je usko vezan s problemom br. 3. Kombinacijom iskustva i provedenih eksperimentalnih ispitivanja, relativne pogreake odreenih mjerenja mogue je tabli no prikazati na sljedei na in (tablica 2-2): Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 2. To nost eksperimentalnih podataka Eksperimentalni podatakProcijenjena to nostNapomenaReferencaTlak zasienja U rasponu 1 barTeake nafte i lagani plinski kondenzati mogu imati i vea odstupanja.Danesh (1998)Z faktor plinaKoriatenjem Standing-Katz dijagrama, to nost u rasponu 1-3%.Standing & Katz (1942)Gustoa stabilizirane (otplinjene) nafteU rasponu 1-3%Danesh (1998)Separatorski volumni faktor nafteU rasponu 2-4%Whitson (2012)Molarna masa stabilizirane (otplinjene) nafte i pseudokomponente (C7+)U rasponu 20%Al-Meshari (2007)Gustoe le~iane nafteEksperimentalno odreene gustoe u rasponu 1-2%.Gustoe nafte iz testa diferencijalnog otparavanja su u rasponu 2-4% (osim zadnjeg koraka!).Drohm et al. (1988)Separatorski proizvodni plinski faktorU rasponu 2%Za lagane plinsko kondenzatne sustave 4-5%Whitson (2012)Proizvodni plinski faktor iz testa diferencijalnog otparavanja (osloboeni plin)U rasponu 3%. Zadnji korak (ispuatanje plina) se ne bi trebao uzimati u obzir! Molni udio C7+ komponente u osloboenim plinovima esto je upitan!Whitson (2012)Sastavi plinova iz testa otparavanja pri stalnom volumenuVisoko kvalitetni laboratoriji trebali bi imati vrijednosti C7+ komponente unutar 1 mol% (metoda kriogene destilacije). Preporu uje se provedba materijalne bilance.Whitson (2012)Kumulativna koli ina proizvedenog plina tijekom testa otparavanja pri stalnom volumenuU rasponu 2-3%Eyton (1987)Omjer kondenzata i plina tijekom testa otparavanja pri stalnom volumenu5-10%Eyton (1987)Udio retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu i otparavanja pri stalnom volumenu5-10%Vee greake mogu se o ekivati za vrlo lagane i fluide blizu kriti ne to ke.Eyton (1987)Relativni volumeni tijekom testa ekspanzije pri stalnom sastavu i otparavanja pri stalnom volumenuU rasponu 5% za hlapive nafte i bogate plinove. Vee greake mogu se o ekivati za vrlo lagane i fluide blizu kriti ne to ke.Danesh (1998)Minimalni tlak mijeaanja U rasponu 5 barWhitson (2012)Viskoznost nafteU rasponu 10-20%Visoka nesigurnost mjerenja!Pedersen et al. (1985)Viskoznost plinaObi no se ne odreuje eksperimentalno Karakterizacija C7+ frakcije Jedan od najte~ih zadataka u PVT karakterizaciji le~ianih fluida je adekvatan opis C7+ frakcije. To se posti~e laboratorijskom karakterizacijom C7+ frakcije, a zatim podeaavanjem parametara jednad~be stanja. Kvalitetna laboratorijska analiza smanjuje potrebu za intenzivnim podeaavanjem parametara jednad~be stanja (Pedersen et al., 1985, Jhaveri & Youngren, 1988, Naji, 2006). Laboratorijska karakterizacija C7+ frakcije Kvalitetna laboratorijska karakterizacija te~ih komponenti uklju uje destilaciju ugljikovodi ne smjese te odreivanje sastava metodom plinske kromatografije ili plinske kromatografije - masene spektrometrije. Destilacija je fizikalna metoda odjeljivanja u procesu kontinuiranog otparavanja komponenata iz smjesa (po etne aar~e), izdvajanja para i njihova kondenzacija kao destilat. Zaostali dio po etnog uzorka je teaki ostatak. Oatrina separacije ovisi o konstrukciji i du~ini destilacione kolone i izra~ava se brojem teoretskih tavana. Teoretski tavan je zamialjeni dio destilacijske kolone na kojem se uspostavlja termodinami ka ravnote~a izmeu plinske i tekue faze. Frakcijska destilacija (engl. true boiling point, TBP distillation) koristi se za izdvajanje grupe frakcije spojeva u zadanom podru ju vreliata. U laboratorijima INA d.d., gdje su raene analize koriatene u disertaciji, destilacija je raena prema standardu ASTM D2892 (ASTM, 2010). Destilacijom se dobivaju frakcije kojima je zatim mogue odrediti molarnu masu, gustou i to ku vreliata ato ini osnovu za procjenu kriti ne veli ine i acentri ne faktore svake pojedine frakcije. Osnovni problem pri provedbi frakcijske destilacije le~ianih ugljikovodika jest potreban volumen fluida-uzorka koji iznosi oko 20 litara. Simulirana destilacija je takoer metoda kojom se mogu odrediti to ke vreliata. Za razliku od fizi ke (frakcijske), simulirana destilacija je br~a i to nija. To nost se u ovom smislu mo~e promatrati kroz parametre ponovljivosti, obnovljivosti i preciznosti (Kriel et al., 1993). Koriatenje simulirane (nasuprot frakcijske destilacije), skrauje vrijeme trajanja karakterizacije C7+ frakcija s nekoliko dana na par sati. Usporedbu rezultata oba tipa destilacije obradili su Kiser & Malone (2006). Zaklju ili su kako se temperature vreliata prosje no razlikuju do maksimalno 5,5C, ato ukazuje na izvrsno uklapanje. Vea razlika primijeena je za viae ugljikovodike. Glavni nedostatak simulirane destilacije je nu~nost procjene molarnih masa i relativnih gustoa pojedina nih frakcija umjesto njihovog eksperimentalnog odreivanja. Grafi ki prikaz krivulje simulirane destilacije dan je na slici 2-17, dok slika 2-18 prikazuje distribuciju frakcija jedinstvenog uglji nog broja odreenih istom metodom.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 17. Krivulja simulirane destilacije  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 18. Distribucija frakcija jedinstvenog uglji nog broja odreenih metodom plinske kromatografije na uzorku kondenzata Metode karakterizacije psudokomponenti za primjenu jednad~bi stanja Najsa~etiju definiciju karakterizacije C7+ frakcije dao je Whitson (1998) definiranjem njezinog cilja:  Jedan od ciljeva C7+ karakterizacije je dobivanje najboljeg mogueg opisa viae stotina nedefiniranih komponenti, koristei minimalan broj pseudokomponenti. U literaturi su dane mnoge procedure za karakterizaciju plus frakcija. Od njih su one predlo~ene od Pedersen et al. (1989) i Whitson et al. (1983, 1989) u najairoj primjeni u naftnoj industriji. Utjecaj razli itih metoda karakterizacije C7+ frakcije opisao je Whitson (1984). Koristei razli ite korelacije za procjenu kriti nih svojstava (tlaka i temperature) doaao je do zaklju ka da imaju veliki utjecaj na predvianje faznog ponaaanja jednad~bom stanja (slika 2-19). Niti jedna od prou enih korelacija, niti njihova kombinacija nisu rezultirale konzistentno boljom jednad~bom stanja (Whitson, 1984) da bi se moglo zaklju iti koju korelaciju treba koristiti.  EMBED Visio.Drawing.11  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 19. Grafi ki prikaz utjecaja razli itih korelacija na predvianje jednad~be stanja (Whitson, 1984) Dva su razli ita pristupa karakterizaciji C7+ frakcije: izravno ra unanje svojstava korelacijama i metoda dijeljenja, nakon dijeljenja ra unanje svojstava (ako nisu poznata) niza novih pseudokomponenti korelacijama i nakon toga grupiranja. Pomou korelacija odreuju se svojstva C7+ frakcije na osnovu relativne gustoe, molarne mase i/ili temperature vreliata. Katz i Firoozabadi (1978) objavili su generalizirani set fizikalnih svojstava za ugljikovodi ne frakcije od C6 do C45. Na osnovu analiza 26 kondenzata i nafti tabli no su prikazali svojstva uklju ujui prosje nu temperaturu vreliata, relativnu gustou i molarnu masu (tablica 2-3). Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 3. Fizikalna svojstva ugljikovodi nih frakcija FrakcijaTb (R)gKMC6606,70,69012,2784C7657,10,72711,9696C8701,70,74911,87107C9747,60,76811,82121C10790,10,78211,83134C11828,60,79311,85147C12866,60,80411,86161C13900,60,81511,85175C14935,20,82611,84190C15970,50,83611,84206C161001,10,84311,87222C171031,70,85111,87237C181055,10,85611,89251C191076,70,86111,91263C201100,10,86611,92275C211123,50,87111,94291C221145,10,87611,95305C231166,70,88111,95318C241186,50,88511,96331C251206,30,88811,99345C261226,10,89212,00359C271245,90,89612,00374C281263,90,89912,02388C291280,10,90212,03402C301294,50,90512,04416C311310,70,90912,04430C321325,10,91212,05444C331339,50,91512,05458C341352,10,91712,07472C351366,50,92012,07486C361379,10,92212,08500C371391,70,92512,08514C381406,10,92712,09528C391418,70,92912,10542C401431,30,93112,11556C411442,10,93312,11570C421452,90,93412,13584C431463,70,93612,13598C441476,30,93812,14612C451487,10,94012,14626 Ahmed et al. (1985) su na osnovu Katz-Firoozabadijevog seta podataka metodom regresije izveli korelaciju slijedeeg oblika:  EMBED Equation.3  (2-30) gdje su:  EMBED Equation.3  fizikalno svojstvo  EMBED Equation.3  broj atoma ugljika (6, 7, & , 45)  EMBED Equation.3  koeficijenti jednad~be dani u tablici 2-4. Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 4. Koeficijenti jednad~be 2-25 (Ahmed et al., 1985)  EMBED Equation.3 a1a2a3a4a5M-131,1137524,96156-0,340790222,494118410-3468,32575Tc (R)915,5374741,421337-0,75868595,867535110-3-1,3028779103pc (psia)275,56275-12,5222690,29926384-2,845212910-31,711722610-3Tb (R)434,3887850,125279-0,90972937,028065710-3-601,85651(-0,508627048,70021110-2-1,848481410-31,466389010-51,8518106(0,867149493,414340810-3-2,83962710-52,494330810-8-1,1627984Vc (ft3/lb)5,22345810-27,8709136910-4-1,932443210-51,754726410-74,401795210-2 Karakterizacija na osnovu korelacija pokazala se neprimjerena za prora une faznog ponaaanja le~ianih fluida (Naji, 2006). Metodom dijeljenja i grupiranja, C7+ frakcija dijeli se na odreen broj pseudokomponenti (naj eae od C7 do C45+, te se za svaku korelacijom odreuju njihova svojstva) te se zatim grupira (na novih nekoliko pseudokomponenata ija se svojstva odrede prema pravilu mijeaanja). Na in dijeljenja i grupiranja predmet je prou avanja stru njaka ve dugi niz godina (Lohrenz et al., 1964, Katz, 1983, Katz & Firoozabadi,1978, Yarbourough, 1979, Whitson, 1983, Pedersen et al., 1984, Whitson, 1989, Nichita et al., 2007, Moradi et al., 2011). Nekoliko autora dokazalo je veliku mogunost pogreanih predvianja faznog ponaaanja le~ianih fluida ukoliko se plus frakcija koristi kao jedna komponenta (Whitson, 1984, Behrens & Sandler, 1986, Pedersen et al., 1989., Danesh, 1998). Komponente le~ianih fluida mogue je podijeliti na (Zuo & Zhang, 2000): Dobro definirane komponente poznatih kriti nih veli ina (temperature i tlaka) te acentri nog faktora. Frakcije jedinstvenog uglji nog broja ije je molarne mase i gustoe mogue eksperimentalno izmjeriti ili odrediti nekom od publiciranih korelacija. Plus frakciju koja se ne mo~e separirati primijenjenom destilacijskom tehnikom. U literaturi postoji zna ajan broj predlo~enih metoda za podjelu C7+ frakcije u pseudokomponente. Za sve vrste dijeljenja moraju biti zadovoljene sljedee pretpostavke: Suma molnih udjela pojedina nih pseudokomponenata jednaka je molnom udjelu C7+ frakcije:  EMBED Equation.3  (2-31) gdje su: zi molni udio komponente i zC7+ molni udio C7+ frakcije Suma produkata molnih udjela i molarnih masa pojedina nih pseudokomponenata jednaka je produktu molnog udjela i molarne mase C7+ frakcije:  EMBED Equation.3  (2-32) gdje su: Mi molarna masa komponente i (g/mol) MC7+ molarna masa C7+ frakcije (g/mol) Suma produkata molnih udjela i molarnih masa podijeljena s relativnom gustoom pojedina nih pseudokomponenata jednaka je onoj od C7+ frakcije:  EMBED Equation.3  (2-33) gdje su: gi relativna gustoa komponente i gC7+ relativna gustoa C7+ frakcije Karakterizacija C7+ uklju uje (Whitson, 2012): korelaciju molarne mase i relativne gustoe C7+ frakcije definiranje trenda i identificiranje zna ajno bitne vrijednosti upotrebu TBP podataka uklapanje s modelom gama distribucije grafi ku korelaciju jedinstvenog uglji nog broja i molarnih masa, odnosno relativnih gustoa kvantitativnu analizu sirove nafte proairenu kromatografsku analizu komponentnog sastava uklapanje s modelom gama distribucije (uz zanemarivanje najte~e, npr. 30+ frakcije). Matemati ki modeli molarne distribucije Kontinuirani distribucijski modeli koriste se za opis molarne distribucije C7+ komponente joa od po etka 1980-ih. Istra~ivanja (Whitson et al., 1986, Sreide, 1989, Whitson et al., 1989, Naji, 2006, Moradi et al., 2011) su pokazala da je za matemati ki opis C7+ frakcija zadovoljavajua eksponencijalna distribucija. Nedostatak upotrebe eksponencijalne distribucije je pretpostavka da sve C7+ frakcije iste molarne mase imaju i jednaku distribuciju, ato nije realno. Model gama distribucije temelji se na gama distribucijskoj funkciji koja je iskrivljena (pomaknuta u jednu stranu) funkcija gustoe vjerojatnosti. Ona stavlja u odnos u estalost pojavljivanja (normalizirani molni udio) i molarnu masu. Whitson (1983) predla~e tri-parametarsku gama funkciju za rjeaenje kontinuirane molarne distribucije:  EMBED Equation.3  (2-34) gdje su: p(M) funkcija gustoe vjerojatnosti M molarna masa koja se koristi kao nezavisna varijabla (g/mol) a, b i h parametri distribucije. Za odreene vrijednosti MC7+, a i h jednad~ba 2-34 predstavlja jedinstveni odnos izmeu normaliziranog molnog udjela i molarne mase C7+ frakcije. Krivulja je definirana od ni~e grani ne vrijednosti (=h) do beskona no. Ukupna povraina ispod krivulje je, po definiciji) jednaka jedan. Kontinuirana distribucija p(M) (odnosno njezin integral, Po(M)) primjenjuje se tako ato se dijeli povraina ispod krivulje kako je prikazano na slici 2-20.  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 20. Molni udio dobiven razlikom povraina ispod funkcije gustoe vjerojatnosti unutar odreenih molnih udjela (Sreide, 1989) Kumulativ funkcije gustoe vjerojatnosti, odnosno njezin integral, predstavlja povrainu ispod krivulje p(M) te izra~ava kumulativ molnih udjela. Kako se krajnja to ka krivulje pribli~ava beskona no, povraina ispod nje se pribli~ava jedan (jednad~ba 2-35).  EMBED Equation.3  (2-35) Behrens & Sandler (1986) predlo~ili su metodu Gaussove kvadrature za rjeaavanje modela kontinuirane molarne gama distribucije s odreenim malim brojem pseudokomponenti. Predlo~eni model dobro aproksimira vrijednosti ukoliko se radi o malom broju pseudokomponenti. Sa veim brojem pseudokomponenti posti~e se bolja integracija povraine distribucije, ali se molarna masa zadnje pseudokomponente poveava do nerealnih veli ina. Da bi se izbjegao taj problem Behrens & Sandler ograni ili su broj pseudokomponenti. Zadovoljavajue rjeaenje seta jednad~bi 2-31 do 2-33, s poativanjem fizikalnih veli ina molarne mase i relativne gustoe pojedinih pseudokomponenti te njihovog proizvoljnog broja, pronaali su Whitson et al. (1989) modifikacijom b parametra u tro-parametarskoj gama funkciji.  EMBED Equation.3  (2-36) Whitson et al. (1989) predla~u metodu za razdjeljivanje C7+ komponente u proizvoljan broj pseudokomponenti koristei Gauss-Laguerreovu kvadraturu i gama distribuciju. Pomou predlo~ene metode mogue je istovremeno izvraiti razdiobu C7+ komponente u viae povezanih fluida. Na taj na in dobivaju se ista kriti na svojstva pseudokomponenti kojima je mogue pridru~iti razli ite molne udjele.  EMBED Equation.3  (2-37) Gdje se te~ine (woi) i nulto ke (xoi) odreuju iz Laguerreovih polinoma. Openito, numeri ka integracija zasniva se na aproksimiranju integrala u kojem su sadr~ane te~ine (woi) i nulto ke (to ke integracije) (xoi). Kod Gaussove kvadrature potrebno je odrediti i te~ine i nulti ke, s time da nulto ke nisu jednako udaljene (ekvidistantne). To ke integracije i te~ine odreuju se pomou ortogonalnih polinoma. Predlo~eni postupak je sljedei (Whitson et al., 1989): Odrediti broj pseudokomponenti N te dobiti vrijednosti Gaussove kvadrature xoi (nulto ke) i woi (te~ine) (tablica 2-5). Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 5. Nulto ke i te~ine za prvih 5 Laguerreovih polinoma (Abramowitz & Stegun, 1965) Nxoiwoi20,5857860,8535533,414210,14644730,4157750,7110932,294280,2785186,289950,010389340,3225480,6031541,745760,3574194,536620,03888799,395070,00053929550,263560,5217561,41340,3986673,596430,07594247,085810,0036117612,64080,00002337 Specificirati h (minimalna mogua molarna masa) koji mora biti jednake vrijednosti za sve C7+ uzoraka. Specificirati o (parametar distribucije) koji mora biti jednake vrijednosti za sve C7+ uzorke. Whitson et al. (1989) predla~u da se za izra unati o koristi molarna masa najte~e komponente MN.  EMBED Equation.3  (2-38) xON je zadnja kvadraturna to ka. Odrediti (na osnovu TBP krivulje) ili procijeniti  vrijednosti ( definira formu distribucije, visinu i airinu) za sve C7+ uzorke. Na osnovu velikog broja eksperimentalnih podataka postoji korelacija izmeu h i  parametara (Sreide, 1989):  EMBED Equation.3  (2-39) Prema Whitsonu (1983) razumne granice za a su izmeu 0,5 i 3,0 dok su prema Sreide (1989) izmeu 0,5 i 1,0. Da bi se zadovoljio uvjet normalizacije (Szi=1), mora se izra unati parametar  za sve C7+ uzorke, pomou jednad~bi:  EMBED Equation.3  (2-40)  EMBED Equation.3  (2-41) , , i h su distribucijski parametri Izra unati molne udjele i molarne mase za sve pseudokomponente pomou jednad~bi:  EMBED Equation.3  (2-42)  EMBED Equation.3  (2-43)  EMBED Equation.3  (2-44) Gama funkcija definirana je sljedeim integralom:  EMBED Equation.3  (2-45) Za ra unalne potrebe koristi se Lanczosova aproksimacija (Lanczos, 1964) ra unanja gama funkcije:  EMBED Equation.3  (2-46) gdje su, p0 = 1,000000000190015 p1 = 76,18009172947146 p2 = -86,50532032941677 p3 = 24,01409824083091 p4 = -1,231739572450155 p5 = 1,20865097386617910-3 p6 = -5,39523938495310-6 To nost Lanczosove aproksimacije, odnosno njezina greaka je manja od 210-10 za sve a>0. Izra unati prosje nu molarnu masu M7+ i provjeriti da li je jednaka eksperimentalno odreenoj vrijednosti. Podeaavati  sve dok nije zadovoljeno slaganje. Za svaki novi  ponovno izra unavati nove molne udjele.  EMBED Equation.3  (2-47) Parametar distribucije h mogue je izra unati sljedeim metodama: Srednja vrijednost izmeu molarne mase frakcije jedinstvenog uglji nog broja najlakae komponente u plus frakciji i prethodne komponente.  EMBED Equation.3  (2-48) Molarne mase frakcija jedinstvenog uglji nog broja uzete su iz tablice 2-3. Ova metoda koristila se tijekom izrade ove disertacije. Jednaka prvoj metodi, osim ato se u prora unu uzimaju molarne mase normalnih parafina.  EMBED Equation.3  (2-49) Molarna masa lakae komponente od one u plus frakciji.  EMBED Equation.3  Molarna masa uzeta iz tablice 2-3. Molarna masa lake komponente od one u plus frakciji, ali jednaka molarnoj masi normalnog parafina.  EMBED Equation.3  U skladu s Whitsonovom preporukom (1983). Gdje je n jedinstveni uglji ni broj plus frakcije (za C7+, n=7).  EMBED Equation.3  (2-50) Jednad~ba stanja Povijesni razvoj jednad~bi stanja Postoji nekoliko vrsti jednad~bi stanja koje mogu opisivati plinske i tekue faze smjese ugljikovodika i ne-polarnih ne-ugljikovodi nih komponenti kao ato su N2, CO2 i H2S. Naj eae se koriste kubne jednad~be stanja, koje se temelje na prvi put predlo~enoj jednad~bi realnog plina od van der Waalsa. Van der Waalsova jednad~ba stanja (1873) bila je prva kojom se moglo predvidjeti istovremeno postojanje plinske i tekue faze. Kasnije su Redlich & Kwong (1949) poveali to nost van der Waalsove jednad~be stanja uvevai temperaturnu ovisnost izraza za privla ne sile (a/V). Soave (1972) modificira Redlich-Kwongovu jednad~bu stanja uvrstivai u nju Pitzerov acentri ni faktor (1955). Peng & Robinson (1976) predla~u svoju jednad~bu stanja temeljenu na istra~ivanju velikog broja sustava prirodnog plina. Nakon tog vremena veliki broj autora bavio se mogunostima poboljaanja kubnih jednad~bi stanja, ali bez nekog zna ajnog rezultata u airoj primjeni za kompleksne spojeve u kojima se za svaki slu aj razlikuje sastav. Kamerlingh Onnes (1901) predlo~io je da se izmjerene vrijednosti korekcijskog faktora za realni plin, Z, prikazuju virijalnom jednad~bom, tj. proairenom izotermnom jednakoau:  EMBED Equation.3  (2-51) gdje su:  EMBED Equation.3  drugi, trei, etvrti, itd. virijalni koeficijenti  EMBED Equation.3  molarni volumen plina (m3/mol) Virijalni koeficijenti B(T), C(T), moraju biti optimalno prilagoeni iskustvenim podacima (p,Vm,T). Obi no se virijalni koeficijenti odreuju metodom najmanjih kvadrata, i to tako da se potra~i polinom najni~ega stupnja koji aproksimira funkciju z(Vm|T) u granicama eksperimentalne pogreake (Butorac & Simeon, 2006). Virijalne jednad~be stanja pokazale su se izuzetno preciznim za potpuno jasan jednostavni sastav (do tri, najviae etiri komponente). Najva~nije prekretnice u razvoju jednad~be stanja grafi ki su prikazane u tablici 2-6. Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 6. Prekretnice u razvoju jednad~be stanja GodinaAutor(i)Doprinos1662.Boylepromjena volumena zraka obrnuto proporcionalna promjeni tlaka pri konstantnoj temperaturi1787.Charleslinearan odnos volumena i temperature pri konstantnom tlaku1801.Daltonzakon parcijalnih tlakova1822.Carniard de la Tourodreivanje svojstava kriti ne to ke1834.Clapeyronzakon idealnog plina1880.Amagatparcijalni volumeni plinova1901.Kamerlingh Onnesvirijalna jednad~ba stanja1940.Benedict et al.osam-parametarska Benedict- Webb-Rubinova JS1949.Redlich & KwongRK JS1955.Martin & Houdetaljna PVT karakterizacija plinova1955.Pitzer et al.acentri ni faktor1972.Soavemodifikacija RK JS, SRK JS1976.Peng & RobinsonPR JS1980.Kumar & Stalingnajopenitija jednad~ba stanja1982.Patel & Tejatri-parametarska JS, proairenje PR JS1982.Peneloux et al.korekcijski parametar volumnog pomaka Kubne jednad~be stanja Prvu kubnu jednad~bu stanja za realne plinove postavio je 1873. godine nizozemski fizi ar Johannes van der Waals. Njegova jednad~ba stanja temelji se na sljedeem modelu: Molekule zauzimaju kona ni molarni volumen, b, tako da plinu ostaje na raspolaganju volumen V-nb i tlak e plina zato biti vei nego kod idealnog plina koji se sastoji od beskona no malih to aka. Privla ne sile proporcionalne su recipro nom molarnom volumenu 1/Vm, odnosno, u estalost udaraca o stjenku proporcionalna je 1/Vm, a isto tako prosje na sila kojom molekula djeluje na stjenku smanjuje se proporcionalno 1/Vm. Ukupno djelovanje molekula na stjenku smanjit e se zato proporcionalno s 1/Vm2 (konstanta proporcionalnosti oznake a). Na temelju tog modela iz jednad~be stanja za idealni plin izvedena je van der Waalsova jednad~ba:  EMBED Equation.3  (2-52) gdje su: p tlak (Pa)  EMBED Equation.3  molarni volumen (m3/mol) R plinska konstanta = 8,3143 (Jmol-1K-1) T temperatura (K) Van der Waalsovi koeficijenti a i b svojstveni su vrsti plina, a neovisni su o temperaturi. U principu to su empirijske konstante pojedinih plinova koje su povezane s meudjelovanjem molekula (a) odnosno s njihovom veli inom i time kona nim volumenom (b). Redlich & Kwong (1949) predlo~ili su unaprijeenu jednad~bu stanja koja je u sebi sadr~avala temperaturnu ovisnost parametra privla nosti molekula a:  EMBED Equation.3  (2-53) gdje su:  EMBED Equation.3  (2-54)  EMBED Equation.3  (2-55) Tc kriti na temperatura (K) pc kriti ni tlak (Pa) Redlich & Kwong su primijetili da ukoliko tlak sustava te~i beskona nom ( EMBED Equation.3 ), molarni volumen tvari smanji se za oko 26% od svog kriti nog volumena ( EMBED Equation.3 ). Redlich-Kwongova jednad~ba stanja se joa uvijek koristi zbog svoje jednostavnosti i fleksibilnosti. No meutim, nije preporu ljiva zbog nepreciznog ra unanja fazne ravnote~e plinska-tekua faza. Acentri ni faktor Acentri ni faktor (w) definirao je Pitzer krivuljom tlaka para pojedine iste tvari (Pitzer et al., 1955). Acentri ni faktor je parametar koji predstavlja nesferi nost molekula i polarnost mnogih komponenti. Jednad~ba stanja idealnih plinova pV=nRT temelji se na modelu vrstih sfera koje se ponaaaju na klasi an i predvidljiv na in. Velika veina tvari je vrlo daleko od idealnog i/ili sferi nog. Acentri ni faktori daju broj koji se koristi u jednad~bi stanja kako bi se JS prilagodila realnom predvianju PVT ponaaanja. Pitzerov acentri ni faktor definiran je jednad~bom:  EMBED Equation.3  (2-56) gdje je:  EMBED Equation.3  tlak para pri temperaturi  EMBED Equation.3  (Tr=0,7) (Pa)  EMBED Equation.3  reducirana temperatura Prakti ki, acentri ni faktor daje mjeru strmosti krivulje tlaka para od Tr=0,7 do Tr=1,0, gdje je  EMBED Equation.3  za  EMBED Equation.3  i  EMBED Equation.3  za  EMBED Equation.3  (slika 2-21).  Slika  STYLEREF 1 \s 2 SEQ Slika \* ARABIC \s 1 21. Acentri ni faktor (Gori nik, 2006) Nakon toga je viae autora (Kesler i Lee, Edmister i drugi) razvilo korelacije za izra unavanje acentri nih faktora ovisno o tipu le~ianog fluida (Whitson & Brul, 2000). Soave (1972) mijenja izraz a/"(T) u Redlich-Kwongovoj jednad~bi stanja funkcijom (T,) uklju ujui temperaturu i acentri ni faktor.  funkcija je prilagoena podacima o tlaku para ugljikovodika tako da ova jednad~ba stanja zadovoljavajue opisuje ugljikovodi ne smjese. Soave-Redlich-Kwongova jednad~ba stanja glasi:  EMBED Equation.3  (2-57) gdje su:  EMBED Equation.3  (2-58)  EMBED Equation.3  (2-59)  EMBED Equation.3  (2-60)  EMBED Equation.3  (2-61) gdje je:  EMBED Equation.3  acentri ni faktor pojedine komponente Soave-Redlich-Kwongovova jednad~ba stanja ne predvia to no faktore kompresibilnosti plina pri kriti nim uvjetima. On se mjeri u rasponu od 0,234 do 0,309 (Vera et al., 1984), dok ga SRK JS predvia kao 0,333. Peng & Robinson (1976) razvili su i objavili novu jednad~bu stanja kako bi zadovoljili sljedee ciljeve: Parametri jednad~be stanja moraju se moi izraziti izrazima kriti nih veli ina i acentri nog faktora. Jednad~ba stanja mora osigurati zadovoljavajuu to nost u blizini kriti ne to ke, naro ito za prora une faktora kompresibilnosti i gustoe tekue faze. Pravilo mijeaanja ne bi trebalo uklju ivati viae od jednog binarnog koeficijenta. Jednad~ba stanja mora se moi primijeniti na svim prora unima svojstava fluida u procesima prirodnog plina. U veem dijelu Peng-Robinsonova jednad~ba stanja daje sli ne rezultate kao i Soave-Redlich-Kwongova jednad~ba stanja, osim ato bolje predvia gustoe tekuina (pogotovo ne-polarnih komponenti) (Firoozabadi, 1988). Peng-Robinsonova jednad~ba stanja (Peng & Robinson, 1976) glasi:  EMBED Equation.3  (2-62) gdje su:  EMBED Equation.3  (2-63)  EMBED Equation.3  (2-64)  EMBED Equation.3  (2-65)  EMBED Equation.3  (2-66) Binarni interakcijski parametar Binarni koeficijenti ili binarni interakcijski parametri (kij) su korekcijski parametri vezani s interakcijom meusobnog privla enja razli itih molekula u realnim smjesama, koji se odreuju na temelju eksperimentalnih podataka o PVT ponaaanju binarnih smjesa (Gori nik, 2006). Binarni interakcijski parametri kij sadr~e odstupanje pojedinog para komponenti (i, j) od ponaaanja idealnih smjesa. Za ugljikovodike do C3 binarni interakcijski parametri imaju vrlo male vrijednosti, tako da je (1-kij=1), dok su vrijednosti interakcijskih koeficijenta za binarne parove viaih ugljikovodika bliske nuli. Kod parova parafini-aromati, parafini (osobito metan)  CO2 ili H2S ili N2, molekulske interakcije su zna ajne tj. vrijednosti kij dovoljno su velike da znatno utje u na to nost rezultata prora una. Zato se tijekom generiranja jednad~be stanja mogu koristiti kao regresijski parametri. Interakcijski koeficijenti odreeni su na temelju eksperimentalnih PVT podataka binarnih smjesa i nisu funkcija p,T i sastava smjese. Preporu eni binarni interakcijski parametri za naj eae koriatene jednad~be stanja u naftnom in~enjerstvu, Peng-Robinsonovu i Soave-Redlich-Kwongovu jednad~bu stanja, dani su u tablici 2-7. Binarni interakcijski parametar definiran je jednad~bom:  EMBED Equation.3  (2-67) gdje je Vc kriti ni molarni volumen. Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 7. Preporu eni binarni interakcijski parametri za Peng-Robinsonovu i Soave-Redlich-Kwongovu jednad~ba stanja Peng-Robinsonova jednad~ba stanja (Nagy & Shirkovskiy, 1982)Soave-Redlich-Kwongova jednad~ba stanja (Reid et al., 1987)N2CO2H2SN2CO2H2SN2------CO20,000--0,000--H2S0,1300,135-0,1200,120-C10,0250,1050,0700,0200,1200,080C20,0100,1300,0850,0600,1500,070C30,0900,1250,0800,0800,1500,070i-C40,0950,1200,0750,0800,1500,060n-C40,0950,1150,0750,0800,1500,060i-C50,1000,1150,0700,0800,1500,060n-C50,1100,1150,0700,0800,1500,060C60,1100,1150,0550,0800,1500,050C7+0,1100,1150,0500,0800,1500,030 Parametar volumnog pomaka Godine 1982. Peneloux et al. uvode korekcijski parametar volumnog pomaka c primijenivi ga na Soave-Redlich-Kwongovu (SRK) jednad~bu stanja na sljedei na in:  EMBED Equation.3  (2-68) gdje su:  EMBED Equation.3  korigirani molarni volumen tekue faze (m3/mol)  EMBED Equation.3  nekorigirani (izra unati) molarni volumen tekue faze (m3/mol)  EMBED Equation.3  molarni udio komponente i u tekuoj fazi (mol)  EMBED Equation.3  koeficijent volumnog pomaka komponente i Usporedba molarnih volumena tekue faze, izra unatih kubnom jednad~bom stanja i odgovarajuih eksperimentalnih podataka, ukazala je na skoro konstantan otklon izra unatih vrijednosti molarnog volumena u odnosu na izmjerene vrijednosti. Posljedica volumnog pomaka je manja izra unata gustoa tekue faze od stvarne (eksperimentalne) gustoe (tablica 2-8). Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 8. Parametri volumnog pomaka istih komponenata za PR JS i SRK JS (Whitson i Brul, 2000) KOMPONENTAPR JSSRK JSciciN2-0,1927-0,0079CO2-0,08170,0833H2S-0,12880,0466C1-0,15950,0234C2-0,11340,0605C3-0,08630,0825i-C4-0,08440,0830n-C4-0,06750,0975i-C5-0,06080,1022n-C5-0,03900,1209n-C6-0,00800,1467n-C70,00330,1554n-C80,03140,1794n-C90,04060,1868n-C100,06550,2080 Jednad~ba stanja le~ianih ugljikovodi nih fluida Za potrebe opisa ponaaanja fluida razvijen je vei broj jednad~bi stanja koje su usporeivali brojni autori Martin (1967, 1979), Abbott (1979), Gray (1979), Yarbourough (1979), Tsonopolous et al. (1985), Firoozabadi (1988), Sreide (1989), Ashour (2011). Abbott je usporedio deset jednad~bi stanja kojima je simulirao laboratorijske eksperimente koji su provedeni na uzorcima iz norveakog dijela Sjevernog mora. Usporedio je njihovu primjenjivost, nedostatke i rezultate. Sreide (1989) daje opairan pregled dvo-, tro- i etvero-parametarskih jednad~bi stanja. Za potrebe svoje disertacije koristio je etvero-parametarsku Martinovu (1979) jednad~bu stanja. Glavni zaklju ak njegove disertacije je da je kvaliteta predvianja faznog ponaaanja le~ianih fluida proporcionalna koli ini i kvaliteti laboratorijske karakterizacije proairenog sastava te~e frakcije, bez obzira koja se jednad~ba stanja koristi. Firoozabadi (1988) usporeuje fazno ponaaanje i volumetrijsko predvianje le~ianih fluida sa Soave-Redlich-Kwongovom (1972), Peng-Robinsonovom (1976) i Schmidt-Wenzelovom (1980) tro-parametarskom jednad~bom stanja. Schmidt-Wenzelova jednad~ba stanja bolje predvia gustoe fluida, dok su prora uni faznih ponaaanja bolji kod Peng-Robinsonove jednad~be stanja (ato potvruje i Ahmedovo istra~ivanje,1986.). Opi zaklju ak dosadaanjih istra~ivanja je da niti jedna jednad~ba stanja nije najpreciznija u predvianju svih potrebnih svojstava, ali da je uz podeaavanje parametara jednad~be stanja mogue relativno to no predviati PVT ponaaanje le~ianih fluida. Ukoliko ne postoje eksperimentalni podaci ponaaanja fluida za promatrano podru je tlakova i temperatura, neophodan je ato bolji  alat za predvianje istog. Podeaavanje parametara jednad~be stanja Za podeaavanje jednad~be stanja potrebno je poznavati kriti ne temperature, kriti ne tlakove i acentri ne faktore pojedinih komponenti. U literaturi postoji niz prijedloga metoda za podeaavanje parametara jednad~be stanja. Vrsta i broj parametara jednad~be stanja koji se mijenjaju (regresiraju/podeaavaju) razli iti su od metode do metode. Aguilar & McCain (2002) predlo~ili su sljedei postupak: Podjela plus frakcije (C7+, C10+, C11+ ili sl.) na grupe jedinstvenog uglji nog broja do C45+ koristei tri-parametarsku gama distribuciju. Molarna masa i temperatura vreliata predlo~eni od Katza i Firoozabadija (tablica 2-3) pridru~uju se svakoj grupi jedinstvenog uglji nog broja. Relativne gustoe ra unaju se za svaku grupu jedinstvenog uglji nog broja pretpostavljajui konstantan Watsonov karakterizacijski faktor (Watson et al., 1935). Kriti na temperatura, kriti ni tlak i acentri ni faktor pridru~uju se svakoj grupi jedinstvenog uglji nog broja koristei najto niju korelaciju. Molarna masa plus frakcije podeaena je tako da reproducira eksperimentalno odreeni tlak zasienja. Grupiranje grupa jedinstvenog uglji nog broja u grupe viaestrukog uglji nog broja (engl. Multi Carbon Number, MCN) i pridru~ivanje kriti nih veli ina svakoj grupi. Posljednji korak je podeaavanje volumetrijskih podataka. Nemogunost kubne jednad~be stanja da reproducira eksperimentalne podatke za ugljikovodi ne le~iane fluida posljedica je dvaju uzroka (Pedersen et al., 1989): pogreaaka uslijed provoenja eksperimentalnih mjerenja: tijekom odreivanja sastava ili volumetrijskih mjerenja, loaeg modela. Podeaavanjem parametara jednad~be stanja mogue je ukloniti taj nedostatak. Parametri regresije Kubne jednad~be stanja ne mogu to no opisivati svojstva i fazno ponaaanje le~ianih fluida bez prilagodbe parametara jednad~be stanja u smislu usklaivanja s eksperimentalno odreenim PVT podacima. Izgec (2003) na nekoliko primjera pokazuje kako Peng-Robinsonova jednad~ba stanja s originalnim vrijednostima pojedinih parametara, ra una tlakove zasienja s pogreakom i do 25% u odnosu na eksperimentalne podatke. Obzirom da ne postoji norma kako i koje parametre jednad~be stanja izabrati za regresiju, to uvelike ovisi o iskustvu in~enjera. Meutim to iskustvo potrebno je preformulirati u statisti ki opravdane smjernice, barem za pojedine vrste fluida. Parametri regresije kubnih jednad~bi stanja mogu biti: kriti na temperatura (Tc), kriti ni tlak (pc), acentri ni faktor ((), binarni interakcijski parametri (kij), parametar volumnog pomaka (c) te potencija (() kod binarnog interakcijskog parametra (Zuo & Zhang, 2000). Coats (1985) predla~e  EMBED Equation.3  i  EMBED Equation.3  parametre metana i najte~ih komponenti te binarne interakcijske koeficijente izmeu metana i najte~e komponente kao standardne regresijske varijable. Ukoliko su ne-ugljikovodi ne komponente CO2 ili N2 prisutne u fluidu u zna ajnoj mjeri, njihovi omega parametri ( EMBED Equation.3  i  EMBED Equation.3 ) se takoer mogu uzeti kao regresijske varijable (Whitson, 1983). Regresija u viae koraka je najbolji na in za odreivanje broja i svojstava pseudokomponenti pomou kojih je mogue kvalitetno opisati le~iani fluid. Koraci regresije ponavljaju se sve dok nije postignuto zadovoljavajue slaganje izmeu izra unatih i eksperimentalnih podataka. Ukoliko nije mogue dobiti dobre rezultate regresijom u viae koraka, preporu a se grupiranje lakaih i srednje-teakih komponenata (N2+C1, CO2+C2, i-C4+n-C4, i-C5+i-C5) te Gaussova kvadraturna raspodjela C7+ frakcije (Whitson, 1983). 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+H*h h>YBj h`ih +EHUjS h`ih +EHUV h`ih +j h`ih +EHUjS h`ih +EHUVh`ih +EHjh`ih +EHU$ºƺȺҺԺܺ޺@D Z\^~>^ <JHTj% hh +EHUjS hh +EHUVhh +EHjhh +EHUh +h5<2 jwh`ih +6h7hUgh`ih +6H*h`ih +6U h`ih +h`ih +H*8z|~bDZVp$gd + t"gd + & F gd & Fgdgd +k, pc) i temperaturom (kriti na temperatura, Tc) pri kojima plinska faza ima jednaka svojstva tekuoj fazi s kojom je u ravnote~i. Jedna od nezavisnih varijabli koje su dio kubi ne jednad~be stanja su kriti na svojstva fluida. Kriti na svojstva smjese ugljikovodika ra unaju se nekim od definiranih pravila mijeaanja. Kriti na svojstva smjese su dakle funkcionalno povezana s poznatim (izmjerenim i publiciranim) kriti nim svojstvima pojedinih komponenata i njihovim molnim udjelima u smjesi. Podeaavanje parametara jednad~be stanja dakle mo~e uklju ivati i podeaavanje kriti nih svojstava onih komponenata za koje ne postoje poznati podaci o kriti nom tlaku i temperaturi, a to su zapravo plus frakcije, tj. pseudokomponente. Analogno, pravilom mijeaanja se ra unski dobivaju i ostala svojstva za smjesu, poput acentri nog faktora (kao estog parametra za izra un tlaka para pojedina ne komponente). Postoji niz korelacija za procjenu kriti nih veli ina ugljikovodi nih frakcija. Veina njih koristi relativnu gustou i temperaturu vreliata kao korelacijske varijable (Whitson, 1984). Prilikom podeaavanja parametara jednad~be stanja na elno je potrebno poativati sljedea pravila (Whitson, 2012): Dobro definirane parametre nije preporu ljivo mijenjati C6- svojstva: M, Tc, pc, ( C6- parametar volumnog pomaka binarne interakcijske parametre izmeu ne-ugljikovodi nih i ugljikovodi nih komponenata C7+ karakterizacija: minimalno 3 pseudokomponente parametri regresije svojstva pseudokomponenata poativati odnos izmeu relativne gustoe, temperature vreliata i molarne mase viskoznosti se podeaavaju na kraju. Edmister (1958) predla~e jednad~bu za acentri ni faktor istih komponenata koja se kroz naredna desetljea dokazala kao vrlo to na za ugljikovodi ne fluide (Danesh, 1998). Ta jednad~ba dovodi u vezu kriti ni tlak (bar), kriti nu temperaturu i temperaturu vreliata.  EMBED Equation.3  (2-69) Riazi i Daubert (1980) predla~u korelaciju koja se koristi za prora un svojstava plus frakcije koriatenjem laboratorijski odreenom molarnom masom i relativnom gustoom te frakcije. Ova korelacija je jedna od naj eae koriatenih u naftnoj industriji. Whitsonovo istra~ivanje (Whitson, 1984) potvruje da je ova korelacija za lakae ugljikovodi ne smjese (koje ne sadr~e komponente vee molarne mase od C25) najto nija i najjednostavnija za upotrebu.  EMBED Equation.3  (2-70) Gdje su:  EMBED Equation.3  fizikalno svojstvo  EMBED Equation.3  koeficijenti za svako pojedino svojstvo (tablica 2-9) Tablica  STYLEREF 1 \s 2 SEQ Tablica \* ARABIC \s 1 9. Koeficijenti za Riazi-Daubertovu korelaciju (Riazi & Daubert, 1980)  EMBED Equation.3 Tc (R)pc (psia)Tb (R)a544,4452036,77857b0,2998-0,80630,401673c1,05551,6015-1,58262d-0,00013478-0,00180780,00377409e-0,61641-0,30842,984036f0,00,0-0,00425288 Riazi & Al Sahhaf (1996) izveli su jednad~bu za ra unanje temperature vreliata, gustoe, kriti nih veli ina, acentri nog faktora i ostalih veli ina grupa jedinstvenog uglji nog broja. Njihova jednad~ba za acentri ni faktor pokazala se kao jedna od to nijih (Al Meshari, 2004):  EMBED Equation.3  (2-71) gdje je Mi molarna masa komponente  i (g/mol). Cavett (1962) daje korelacije za kriti ne veli ine tlaka (2-69) i temperature (2-70) ugljikovodi nih frakcija koje se temelje na polinomu drugog stupnja temperature vreliata i gustoe izra~ene u stupnjevima API svake komponente. Arbabi i Firoozabadi (1995) napravili su usporedbu kriti nih tlakova i temperatura normalnih alkana od heptana do tetrakontana. Kriti ne veli ine izra unate su pomou etiri korelacije: Cavett, Kesler-Lee, Twu, i Riazi-Daubert. Tvrde da je Cavettova korelacija najto nija pri procjeni kriti nih veli ina.  EMBED Equation.3  (2-72)  EMBED Equation.3  (2-73) gdje su: pci kriti ni tlak komponente i (psia) Tci kriti na temperatura komponente i (R) Tbi temperatura vreliata komponente i (R) APIi gustoa komponente i ( EMBED Equation.3 ) Tridesetih godina proalog stoljea uo ena je obrnuta proporcionalnost omjera atoma vodika i ugljika (H/C omjer) i relativne gustoe. Takoer, uo ena je funkcionalna ovisnost broja ugljika i temperature vreliata. Doti ne funkcionalne veze mogu se izraziti Watsonovim faktorom (1935). Pretpostavljajui Watsonov karakterizacijski faktor ( EMBED Equation.3 ) konstantan za svaku frakciju, mogue je izra unati relativnu gustou iz jednad~be 2-66 (Whitson, 1983):  EMBED Equation.3  (2-74) Potrebno je izabrati Watsonov karakterizacijski faktor kojim se izra una relativna gustoa plus frakcije, eksperimentalno odreena vrijednost.  EMBED Equation.3  (2-75) gdje su: g7+ relativna gustoa C7+ frakcije M7+ molarna masa C7+ frakcije (kg/kmol) x7+ molni udio C7+ frakcije (mol/mol) gi relativna gustoa frakcije i Mi molarna masa frakcije i (kg/kmol) xi molni udio frakcije i (mol/mol) Takoer, potrebno je da  EMBED Equation.3  zadovolji sljedei kriterij:  EMBED Equation.3  (2-76) Gdje je:  EMBED Equation.3  (2-77) Izra unavai  EMBED Equation.3  i  EMBED Equation.3 , temperatura vreliata pojedine pseudokomponente izra una se iz jednad~be (Watson et al., 1935):  EMBED Equation.3  (2-78) Korelaciju za odreivanje kriti nih veli ina temperature, tlaka i volumena koriatenu tijekom izrade disertacije izveo je Twu (1984). Korelacija za naftne frakcije ra una se pomou primarno odreenih korelacija za normalne parafine. Korelacije za normalne parafine (Twu, 1984):  EMBED Equation.3  (2-79)  EMBED Equation.3  (2-80)  EMBED Equation.3  (2-81)  EMBED Equation.3  (2-82)  EMBED Equation.3  (2-83) gdje su: Tcp kriti na temperatura normalnih parafina (R) Tb temperatura vreliata (R) pcp kriti ni tlak normalnih parafina (psia) Vcp kriti ni volumen normalnih parafina (ft3/lbm mol)) gp relativna gustoa normalnih parafina Korelacija za kriti nu temperaturu (Twu, 1984)  EMBED Equation.3  (2-84) gdje je: Tc kriti na temperatura (R) Tcp kriti na temperatura normalnih parafina (R)  EMBED Equation.3  (2-85)  EMBED Equation.3  (2-86) Korelacija za kriti ni volumen (Twu, 1984)  EMBED Equation.3  (2-87) gdje je: Vc kriti ni volumen (ft3/lbm mol)) Vcp kriti ni volumen normalnih parafina (ft3/lbm mol))  EMBED Equation.3  (2-88)  EMBED Equation.3  (2-89) Korelacija za kriti ni tlak (Twu, 1984)  EMBED Equation.3  (2-90) gdje je: pc kriti ni tlak (psia) pcp kriti ni tlak normalnih parafina (psia)  EMBED Equation.3  (2-91)  EMBED Equation.3  (2-92) Obrada podataka istra~ivanja Statisti ka obrada podataka Kvaliteta jednad~be stanja, odnosno usporedba rezultata pojedinih eksperimentalnih testova i podataka reproduciranih odreenom jednad~bom stanja, tj. matemati ki simuliranih testova, pri istim uvjetima, provjeravana je metodom odstupanja zbroja kvadrata ponderiranih rezidualnih odstupanja. Metoda najmanjih kvadrata odstupanja temelji se na na elu da su najbolje odreeni parametri neke funkcije, za koje je suma kvadrata odstupanja izmeu mjerenih vrijednosti i vrijednosti izra unatih tom funkcijom minimalna. Promatranje sume razlika eksperimentalnih i izra unatih podataka, nije prihvatljivo jer se pozitivne i negativne razlike poniatavaju. Objektivni kriterij usklaenosti neke funkcije s eksperimentalnim ili referentnim podacima je svoenje sljedeeg izraza na minimum:  EMBED Equation.3  2-93 gdje su:  EMBED Equation.3  zbroj kvadrata ponderiranih rezidualnih odstupanja  EMBED Equation.3  rezidualno odstupanje izmeu mjerene (eksperimentalno odreene) vrijednosti i te pripadajueg predvianja jednad~bom stanja  EMBED Equation.3  ponderacijski faktor za rezidualno odstupanje  EMBED Equation.3  Rezidualna odstupanja ra unaju se kao relativni postotci jednad~bom:  EMBED Equation.3  2-94 gdje su:  EMBED Equation.3  izra unata vrijednost opa~anja i  EMBED Equation.3  eksperimentalna vrijednost opa~anja i  EMBED Equation.3  referentna vrijednost opa~anja i Za pojedino izdvojeno mjerenje kao ato je odreivanje tlaka zasienja le~ianog fluida, referentna vrijednost bit e jednaka eksperimentalno odreenoj vrijednosti, odnosno vrijedit e:  EMBED Equation.3 . Ukoliko je mogue odrediti standardnu devijaciju (uvjetovano brojem odreenih vrijednosti), ponderacijski faktori su obrnuto proporcionalni standardnoj devijaciji, odnosno mogu se izra unati prema jednad~bi:  EMBED Equation.3  2-95 gdje je:  EMBED Equation.3  standardna devijacija opa~anja i U tom slu aju kombinacijom jednad~bi 2-93 i 2-95, dobivamo jednad~bu za ra unanje zbroja kvadrata ponderiranih rezidualnih odstupanja vezanu za standardnu devijaciju mjerenja:  EMBED Equation.3  2-96 U slu ajevima kada nije mogue odrediti standardnu devijaciju, pretpostavljeni ponderacijski faktori jednaki su 1, ukoliko se ne zada druga ije. Tako na primjer Danesh (1998) preporu a ponderacijski faktor 40 za tlak zasienja, 20 za gustou, 10 za volumen i 1 za sastav. Naime, utjecaj varijable na koju se podeaavaju parametri jednad~be stanja poveava se sa sve viaim ponderacijskim faktorom. Tlak zasienja je jedno od najva~nijih svojstava le~ianih fluida te mu je zato preporu ljivo dati visok ponderacijski faktor. S druge strane, potrebno je biti svjestan to nosti odreenog tlaka zasienja budui da on direktno utje e na predvianje volumena retrogradnog kondenzata. Za pravilnu upotrebu ponderacijskih faktora, bitno je dobro poznavanje metoda koje se primjenjuju u laboratorijskom ispitivanju le~ianih fluida te povjerenje prema laboratoriju koje provodi testove. Razine eksperimentalnih pogreaaka koje se trebaju uzeti u obzir prethodno su prikazane u tablici 2-2. Budui da su ponderacijski faktori proizvoljni, nije mogue dodijeliti jednozna no zna enje izrazu  EMBED Equation.3 . Zbog tog razloga neke PVT ra unalne aplikacije, kao ato je PhazeComp, daju izvjeataj pogoenosti regresije u obliku koji je povezan s  EMBED Equation.3 , ali ga je lakae interpretirati:  EMBED Equation.3  2-97 gdje je:  EMBED Equation.3  kvadratna sredina rezidualnih odstupanja. Grafi ka obrada podataka esto je grafi ka vizualizacija bolje rjeaenje za promatranje usklaenosti odreenih setova podataka. Tu tvrdnju mogue je konkretno razmotriti u kontekstu usporedbe koja jednad~ba stanja bolje opisuje promatrani uzorak. Na primjer, kod prora una testa separacije usporeuju se etiri eksperimentalno odreena parametra (plinske faktore i gustoe tekue faze pri prvom i drugom testu separacije) s pripadajuim vrijednostima izra unatim jednad~bama stanja. Ukoliko se vrijednostima u statisti ku obradu ne uklju e odgovarajui ponderacijski faktori (najbolje bi bilo da su oni odreeni standardnim devijacijama pojedinog mjerenja), rezultati sume najmanjih kvadrata i/ili kvadratna sredina rezidualnih odstupanja mogu zaklju ak odvesti u pogreanom smjeru. To je posebice izra~eno kod plinskih kondenzata. Naime, plinski faktori mogu biti izrazito veliki u usporedbi s gustoama, a razina pouzdanosti njihovog odreivanja je puno manja. Tako da ukoliko bi se uzimao pretpostavljeni ponderacijski faktor 1 za sve promatrane vrijednosti, puno veu te~inu bi imalo odstupanje proizvodnog plinskog faktora, a ne eksperimentalno odreena gustoa otplinjenog kondenzata ije je mjerenje to nosti na razini 1%. EKSPERIMENTALNO ISTRA}IVANJE Uzorci Uzorci le~ianih fluida ispitani i obraeni za potrebu disertacije, uzorkovani su u razdoblju od 2003. do 2011. godine. Ukupno je uzorkovano 40 uzoraka (slika 3-1) ugljikovodi nih fluida s 5 polja, odnosno iz 5 le~iata i 11 buaotina. Uzorkovani su separatorski i dubinski uzorci. Na njima su izvraena brojna PVT ispitivanja uklju ujui: utvrivanje tla no volumnih odnosa te kontaktno otplinjavanje separatorske nafte/kondenzata (26 uzoraka), kromatografske analize separatorskih fluida (svi uzorci), odreivanje gustoe stabilizirane nafte/kondenzata (svi uzorci), frakcijsku destilaciju nafte/kondenzata u svrhu karakterizacije pseudokomponente (C7+) (26 uzoraka), prora un sastava ukupnog proizvedenog buaotinskog fluida (26 uzoraka), test ekspanzije pri konstantnom sastavu (20 uzoraka), test otplinjavanja pri konstantnom volumenu (12 uzoraka), diferencijalno otplinjavanje (8 uzoraka), separator test (3 uzorka), te viskoznost (7 uzoraka) i gustoa fluida pri le~ianim uvjetima (8 uzoraka). Tabli ni prikaz izvraenih analiza na ispitivanim uzorcima dan je u tablici 3-1.  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 1. PVT spremnici sa separatorskim uzorcima Tablica  STYLEREF 1 \s 3 SEQ Tablica \* ARABIC \s 1 1. Izvraene analize `ifra uzorkaIntervalTip fluidaIzvraene analizeNapomenaSastavFlashCCECVDDLViskoznostA-6-12960-2901kond.XXkontaminirano uljnom isplakomA-2-1,2,3,43633--3553kond.X4 DST uzorkaA-4-13326-3242.5naftaXDST uzorakA-2-53019-3020kond.XXX / 5XMDTA-1-13035-2906kond.XXA-1-23035-2906kond.XXX / 4XA-2-63790--3756kond.XXX / 5XA-2-73633--3443kond.XXA-6-23516--3332kond.XXX / 5XA-2-83633--3553kond.XXA-2-93390--3380kond.XXX / 5XA-2-103332--3278kond.XXA-2-113332--3278kond.XXA-2-123109--3096naftaXXX / 1XXA-2-133074--3055naftaXXX / 1XX`ifra uzorkaIntervalTip fluidaIzvraene analizeNapomenaSastavFlashCCECVDDLViskoznostA-2-143026--3016kondXXX / 5XA-6-33125--3096naftaXXA-2-153026-2919kondXXX / 5XA-2-163026-2919kondXXA-2-173109--3096naftaXXX / 1XA-1-32832,6 2839,5kondXXX / 5XB-1-13450 -- 3429naftaXXX / 1Xuklanjan viaak plinaB-2-13409-3441naftaXXX / 3XX+separator testB-2-23505-3508naftaXXX / 3XX+separator testC-1-13118-3074naftaXXX / 1XXC-1-23443--3435naftaXXC-1-33443--3435naftaXXX / 1XXC-3-13031--3009naftaXXX / 4XD-1-12094.5--2050naftaXXX / 3XX+separator test `ifra uzorkaIntervalTip fluidaIzvraene analizeNapomenaSastavFlashCCECVDDLViskoznostE-1-12235--2221kondXXX / 5XE-1-2,3kondX2 DST uzorkaE-2-1samo plinX1 DST plinE-2-22469--2439kondXE-2-32049-2301kondXXX / 4XE-1-42402-2219kondXX Instrumentacija i programska podraka Analiza sastava i svojstava plina i nafte/kondenzata Plinska faza analizirana je na Agilentovom plinskom kromatografu tipa 6890N konfiguriranom za proairenu kromatografsku analizu u skladu s normom HRN EN ISO 6975:2008 Prirodni plin -- Proairene analize -- Metoda plinske kromatografije. Kolone instalirane na plinskom kromatografu (slika 3-2) za odreivanje komponentnog sastava plinske faze su: kolona 1: Hayesep Q 80/100 mesh 3 ft 1/8 in (analiza CO2, C2) kolona 2: referentna Hayesep Q 80/100 mesh 6 ft 1/8 in kolona 3: Molecular Sieve 13 X, 45/60 mesh 10 ft 1/8 in (analiza O2, N2 i C1) kolona 4: 50m 200m 0,5m PONA (analiza C3, i-C4, n-C4, i-C5, n-C5, od C6 do C14)  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 2. Plinski kromatograf za analizu plinske faze Temperaturni program za koriatenu metodu dan je u tablici 3-2. Tablica  STYLEREF 1 \s 3 SEQ Tablica \* ARABIC \s 1 2. Temperaturni program metode za analizu plinske faze KorakRast temperature C/minCiljana temperatura CIzotermno minVremenska tablica min1.6010102.152001736,33Analize tekuih ugljikovodi nih fluida analizirane su u skladu s metodom ASTM  Standard D 2887 (2008). Plinski kromatograf Agilent 6890N (slika 3-3) za simuliranu destilaciju tj. distribuciju ugljikovodika prema vreliatu u frakcijama nafte i kondenzata sastoji se od sljedeih dijelova: Visoko rezolutna kapilarna kolona za plinsku kromatografiju sljedeih karakteristika: tip kolone: HP-5MS duljina: 60 m promjer kapilare: 0,32 mm debljina filma: 0,25 m temperaturni raspon od -60C do 350C Termostat (pe) s mogunoau programiranja temperature, u kojoj je smjeatena kolona. Temperaturni program za koriatenu metodu dan je u tablici 3-3. Elektronska kontrola tlaka koja omoguava stalan protok plina nosioca kroz kolonu i ponovljivost vremena zadr~avanja Automatski injektor za ubacivanje uzorka pri atmosferskom tlaku. Injektirani volumen uzorka iznosi 1l, s time da je split odnos 10:1 uz protok plina nosioca (helija) od 17,9 ml/min. Ra unalo s programom koji omoguava potpunu kontrolu zadanih uvjeta za kromatografsku analizu (za odabranu metodu), ra unsku obradu i ispis rezultata analize Izvor plinova potrebnih za kromatografsku analizu i paljenje detektora: plin nosilac (helij)  plinska boca s regulatorom i indikatorom tlaka zrak (iz sistema ili boce)  s regulatorom tlaka vodik  plinska boca vodika s regulatorom tlaka ili generator vodika duaik  plinska boca duaika s regulatorom tlaka. Plameno ionizacijski detektor. Tablica  STYLEREF 1 \s 3 SEQ Tablica \* ARABIC \s 1 3. Temperaturni program metode za analizu tekueg ugljikovodi nog fluida KorakRast temperature C/minCiljana temperatura CIzotermno minVremenska tablica min1.3510102.1400153.8150028,754.103504088,75  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 3. Plinski kromatograf za analizu tekue faze Kontaktno otplinjavanje separatorske nafte/kondenzata Kontaktno otplinjavanje provodilo se u PVT elijama proizvoa a Ruska, Core Laboratories i IMG. Zaporni volumeni elija iznose izmeu 500 i 600 cm3. Tla ni medij je ~iva. elije su konstruirane za radne temperature od 20C do 150C, te radne tlakove do 700 bar. Tijekom procesa otplinjavanja pomoni instrumenti bili su: trap za hlaenje kivete u kojoj se sakuplja otplinjena tekua faza, kiveta, analiti ka vaga te plinomjer (slika 3-4).  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 4. Kontaktno otplinjavanje separatorske nafte Rekombinacija Rekombinacija le~ianog fluida vraila se u eliji za rekombinaciju (slika 3-5). elija za rekombinaciju konstruirana je kao prolazna elija s dva T ventila na vrhu i dnu. Prije same rekombinacije elija je bila o iaena (aromatskim otapalima), osuaena (aceton, grijanje, propuhivanje inertnim plinom helijem) te vakuumirana. Unutarnji volumen elije iznosi dvije litre, tako da je bilo mogue jednokratno rekombinirati le~iani fluid koji e se koristiti za sve daljnje analize.  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 5. elija za rekombinaciju Test ekspanzije pri stalnom sastavu Test ekspanzije pri stalnom sastavu provodio se na instrumentu 3000 PVT Phase Behavior System (slika 3-6), proizvedenom od strane kompanije Chandler Engineering. Model 3000 PVT Phase Behavior System sastoji se od dvije termostatirane elije od kojih je jedna plinsko-kondenzatna, a druga naftna elija. Obje elije omoguavaju vizualno detektiranje tlaka rosiata, odnosno tlaka isparavanja te praenje retrogradne kondenzacije i odnosa faza. Zaporna tekuina u cijelom ureaju (elija i pumpa) je hidrauli ko ulje. Ureaj se sastoji od termostata, visokotla ne volumetrijske uljne pumpe i kontrolnog pulta. Maksimalni radni tlak naftne elije je 1040 bar, a plinsko kondenzatne elije 1380 bar. To nost o itanja tlaka prema specifikaciji instrumenta iznosi 0,1% pune skale. Maksimalna radna temperatura iznosi 204C, s to noau regulacije 0,5C (Chandler, 2005). To nost o itanja volumena fluida iznosi 0,1cm3, a o itanja volumena retrogradnog kondenzata 0,01 cm3 (Chandler, 2005).  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 6. Instrument 3000 PVT Phase Behavior System Diferencijalno otparavanje Diferencijalno otparavanje provodilo se na instrumentu 3000 PVT Phase Behavior System (slika 3-6). Separator test Separator testovi provodili su se na instrumentu 2353-805 Equilibrium Flash Separator od Chandler Engineering-a (slika 3-7). Maksimalni radni tlak instrumenta iznosi 34,5 bar pri 93,3C (Chandler, 2008).   Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 7. Instrument za provedbu separator testa model 2353-805 Equilibrium Flash Separator Viskoznost Eksperimentalno odreivanje viskoznosti le~iane nafte vrailo se pomou viskozimetra s rotirajuom kuglicom proizvoa a ROP. Ureaj za mjerenje viskoznosti fluida pri le~ianim uvjetima (slika 3-8) sastoji se od: ROP viskozimetra visokotla ne volumetrijske pumpe (tla ni medij ~iva) termostata. Odreivanje viskoznosti fluida sastojalo se od mjerenja vremena potrebnog da kuglica proe odreeni put kroz cijev, napunjenu fluidom i nagnutu pod poznatim kutom. Vrijeme prolaza kuglice proporcionalno je: viskoznosti fluida, kutu nagiba cijevi (22, 45 ili 70), gustoi kuglice te gustoi fluida u kalibriranoj cijevi kod radnog tlaka i temperature.  EMBED CDraw5 \* MERGEFORMAT  Slika  STYLEREF 1 \s 3 SEQ Slika \* ARABIC \s 1 8. Shematski prikaz viskozimetra s rotirajuom kuglicom Viskoznosti le~ianih fluida podeaavane su na kraju karakterizacije. Lohrenz-Bray-Clarkova korelacija koriatena je za ra unanje viskoznosti le~ianih fluida (jednad~ba 4-13) (Lohrenz et al., 1964). Regresija je vraena modifikacijom kriti nih volumena pseudokomponenata. Posebna pa~nja posveena je provjeri koeficijenata polinoma LBC korelacije budui da je potrebno osigurati monotonost viskoznosti i pojedinih frakcija.  EMBED Equation.3  (4-13) gdje su:  EMBED Equation.3  (4-14)  EMBED Equation.3  viskoznost komponente i (mPas)  EMBED Equation.3  molni udio komponente i  EMBED Equation.3  molarna masa komponente i (kg/kmol)  EMBED Equation.3  (4-15)  EMBED Equation.3  Thodosov korelacijski parametar (mPas-1)  EMBED Equation.3  (4-16) Test otparavanja pri stalnom volumenu Test otparavanja pri stalnom volumenu provodilo se na instrumentu 3000 PVT Phase Behavior System (slika 3-6). Laboratorijska karakterizacija C7+ frakcije Laboratorijska karakterizacija C7+ frakcije sastojala se od: atmosferske destilacije stabilizirane tekue faze (nafte/kondenzata); kromatografske analize, odnosno simulirane destilacije C7+ frakcije te eksperimentalnog odreivanja gustoe C7+ frakcije. Atmosferska destilacija provodila se u skladu s normom ASTM  Standard D 2892-90, Standard Test Method for Distillation of Crude Petroleum. Simulirana destilacija vraila se metodom plinske kromatografije na instrumentu Agilent Technologies 6890N (Agilent, 2005) u skladu s normom ASTM D2887 - 08 Standard Test Method for Boiling Range Distribution of Petroleum Fractions by Gas Chromatography. Gustoa je mjerena na instrumentu DA-505 u skladu s normom ASTM D5002 - 99(2010) Standard Test Method for Density and Relative Density of Crude Oils by Digital Density Analyzer. Programska podraka U radu je koriatena aplikacija PVTp razvijena od kompanije Petroleum Experts (Petex) iji se paket koristi u INA d.d. PVTp je aplikacija za karakterizaciju le~ianih fluida jednad~bom stanja. Na tr~iatu postoji viae PVT aplikacija za uklapanje laboratorijskih podataka u jednad~bu stanja. Svaka od navedenih aplikacija ima svoje specifi nosti koje se temelje na razli itim korelacijama i algoritmima. PVTp kao aplikacija ima svoje nedostatke, kao ato su karakterizacija psudokomponente i nemogunost istovremene obrade dva ili viae razli itih uzoraka le~ianih fluida. Tip le~ianog fluida (nafta ili kondenzat) ima izra~en utjecaj na trajanje i samu mogunost regresije zadanih parametara jednad~be stanja. Kondenzatni se fluidi zbog svoje kompleksnije prirode ponaaanja (retrogradna kondenzacija, retrogradna evaporacija, vea koli ina srednje teakih komponenata koje imaju sli ne sklonosti biti e u obje faze u airem rasponu tla no-temperaturnih uvjeta) puno te~e uklapaju od naftnih fluida. Tako da ukoliko se radi s kondenzatnim fluidima, nije preporu ljivo istovremeno razmatrati viae od dva uzorka. Ukoliko se radi samo s naftnim fluidima, broj uzoraka koji se istovremeno obrauje mo~e biti i vei. U sklopu PVTp-a koristi se Whitsonova metoda za dijeljenje pseudokomponente temeljena na radu iz 1983. godine (Whitson, 1983). S obzirom da je dokazano to nija metoda dijeljenja Gaussova kvadraturna metoda (Whitson et al., 1989) napravljena je aplikacija u excelu temeljena na toj metodi. U tablici (3-4) dan je prikaz rada te aplikacije na primjeru jednog od uzoraka obraenih u ovome radu. Tablica  STYLEREF 1 \s 3 SEQ Tablica \* ARABIC \s 1 4. Dijeljenje C7+ frakcije modificiranom Whitsonovom metodom (1989) EKSPERIMENTALNI PODACILITERATURARA UNIZRA UNATI REZULTATI MC7+=159,33gC7+=0,78676zC7+=0,03149N=5h=90bO=32,434656a=1=1,00Cf=0,27662421 PseudoxOnwOnzOnMwnf(xOn)gOnTbnbr.mol%kg/kmolC10,263560,5217560,884598,550,5382720,72053101,9721,41340,3986671,2462135,840,9925470,765926166,5933,596430,0759420,7586206,653,1716810,811696266,1147,085810,0036120,2310319,8320,311860,853672381,05512,64082,34E-050,0287500,00390,49060,894706501,67 PseudoTbTcPagPgDgTfTTcbr.RR1675.217443979.940.31100.691280.72053-0.136050.00196995.42791.525311100.540.28080.729760.76593-0.165440.0022991121.03970.6619071266.950.23390.770150.81170-0.187580.0025131292.741177.560561436.250.18010.800770.85367-0.232430.0031141472.551394.679751595.390.12580.820720.89471-0.309230.0043821652.3 PseudovcPDgvfvvcpcPDgpfppcbr.ft3/lbm molft3/lbm molpsiapsia16,92-0,1522-0,00436,6876393,0-0,01450,00154418,229,28-0,1946-0,00618,8358315,6-0,01790,00197342,8314,09-0,2312-0,008013,2101220,9-0,02060,00347247,1421,78-0,2954-0,012319,7412141,8-0,02610,00741170,2532,61-0,3981-0,021127,548385,5-0,03630,01579118,9 PseudoTbrKwwwbr.10,67812,1760,1904990,308920,70612,0770,3545540,410330,75112,1980,6135460,604940,799712,3700,9071580,875450,84412,4881,1866921,2046 Za ra unanje w koriatena je Lee-Keslerova korelacija (Lee & Kesler, 1975): Za  EMBED Equation.3   EMBED Equation.3  (4-11) gdje su A1=-5,92714, A2=6,09648, A3=1,28862, A4=-0,169347, A5=15,2518, A6=-15,6875, A7=-13,4721, A8=0,43577 Za  EMBED Equation.3   EMBED Equation.3  (4-12) REZULTATI ISTRA}IVANJA Provjera podataka koji prethode laboratorijskim PVT ispitivanjima Izvraena je kontrola kvalitete svih PVT podataka. U tom smislu napravljeno je: Utvrivanje reprezentativnosti uzorka, grafi ki je provjereno slaganje relativne gustoe i molarne mase C7+ frakcije separatorskog kondenzata/nafte (tablica 4-1, slika 4-1), provjeren je Watsonov karakterizacijski faktor za separatorsku tekuu fazu (tablica 4-1, slika od 4-2 do 4-5), grafi ki je prikazan odnos molnog udjela na logaritamskoj skali obzirom na jedinstveni uglji ni broj u uzorku separatorskog kondenzata/nafte na linearnoj skali za odabrane setove podataka (Prilog I: tablica 1, slike od 4-6 do 4-10), napravljena je provjera K omjera od metana do heksana pri uvjetima separacije na polju koriatenjem Hoffman-Crump-Hocott metode te usporedba linearnog trenda s vrijednostima Standingove korelacije za odabrane setove podataka (Prilog I: tablice od 2 do 6, slike od 4-11 do 4-15). Obzirom da ta metoda uzima u obzir separatorske uvjete (tlak i temperaturu) te eksperimentalno odreene sastave separatorskih uzoraka, ovim na inom se provjeravaju to nost dobivenih separatorskih i proizvodnih podataka, kvaliteta odreivanja sastava te stabilnost separatorskih fluida tijekom uzorkovanja. Tijekom izrade rada izvraena su brojna ispitivanja na svim uzorcima. Neki od uzoraka nisu bili pogodni za provedbu svih PVT ispitivanja budui da nisu adekvatno uzorkovani (na pr. uzorci uzorkovani tijekom DST-a). Prilikom nekoliko uzorkovanja zabilje~eni su nestabilni uvjeti rada separatora, ili preveliki pad tlaka na dnu buaotine. Takvi uzorci smatraju se nereprezentativnim, odnosno nije ih preporu ljivo uzeti u daljnje promatranje za karakterizaciju le~iata ukoliko postoje drugi, reprezentativni uzorci. S obzirom da je tijekom izrade ovog rada bio dostupan dovoljan broj reprezentativnih uzoraka za svako promatrano le~iate, nereprezentativni uzorci su koriateni samo kao eventualna dodatna provjera jednad~be stanja podeaene na reprezentativne uzorke. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 1. Podaci za C7+ frakcije analiziranih uzoraka. Izabrani reprezentativni uzorci za pojedino polje su osjen ani. `ifra uzorkaMolarna masa (kg/kmol)Relativna gustoaKwA-1-3167,270,793212,06A-1-2144,390,775412,02A-2-6166,250,790012,09A-2-9160,600,786812,07A-2-14165,270,789712,08A-2-15156,820,786112,03A-6-2163,350,787512,09A-2-12237,570,849512,00A-2-13240,940,852311,99A-2-17225,410,841212,01B-1-1192,070,807412,13B-2-2211,370,825712,08C-1-1224,590,854811,84C-1-2224,580,850711,89C-1-3220,910,851111,85C-3-1220,420,852811,75D-1-1195,520,846811,68E-1-1128,040,763911,95E-2-3134,040,766312,01 Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 1. Grafi ki prikaz molarne mase u odnosu na relativnu gustou C7+ frakcija analiziranih uzoraka  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 2. Grafi ki prikaz Watsonovog karakterizacijskog faktora analiziranih uzoraka  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 3. Provjera Watsonovog karakterizacijskog faktora za polje A. Izabrani reprezentativni uzorci A-2-9 i A-2-17 zaokru~eni su crvenom kru~nicom. Ostali uzorci na grafu su iz istog le~iata, ali uzorkovani pod razli itim proizvodnim uvjetima (razli iti promjeri sapnica, razli iti separatorski uvjeti). Srednja vrijednost Watsonovog karakterizacijskog faktora iznosi 12,04 (na slici prikazano crtkanom crvenom linijom). Za svaku to ku prikazana su dozvoljena odstupanja po Gori niku (2004). Vidljivo je da promatrani uzorci zadovoljavaju ovaj kriterij reprezentativnosti. Kona ni odabir najreprezentativnijih uzoraka temeljen je prema broju provedenih PVT ispitivanja i prema kvaliteti uvjeta pri kojima je uzorkovano.  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 4. Provjera Watsonovog karakterizacijskog faktora za polje B. Srednja vrijednost Watsonovog karakterizacijskog faktora iznosi 12,10 (na slici prikazano crtkanom crvenom linijom  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 5. Provjera Watsonovog karakterizacijskog faktora za polje C. Srednja vrijednost Watsonovog karakterizacijskog faktora iznosi 11,85 (na slici prikazano crtkanom crvenom linijom  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 6. Provjera kvalitete sastava uzorka A-2-9: odnos molnog udjela na log skali i jedinstvenih uglji nih brojeva. U usporedbi s eksponencijalnom funkcijom promatranog sastava (crvena linija), mogue je zaklju iti da je sastav frakcije korektno odreen. Mala odstupanja unutar su analiti ke pogreake predviene koriatenom metodom plinske kromatografije (ASTM  Standard D 2887, 2008).  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 7. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka A-2-17  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 8. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka A-1-2  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 9. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka E-2-3  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 10. Odnos molnog udjela i jedinstvenih uglji nih brojeva uzorka C-3-1  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 11. Grafi ki prikaz HCH/Standing korelacije za uzorak A-2-9  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 12. Grafi ki prikaz HCH/Standing korelacije za uzorak A-2-17  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 13. Grafi ki prikaz HCH/Standing korelacije za uzorak C-3-1  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 14. Grafi ki prikaz HCH/Standing korelacije za uzorak E-2-3  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 15. Grafi ki prikaz HCH/Standing korelacije za uzorak A-1-2 Podaci laboratorijskih PVT ispitivanja i njihova provjera U Prilogu I u tablicama od 7 do 28 dani su podaci laboratorijskih analiza koji su ulazni podaci za podeaavanje parametara jednad~be stanja. Redom su prikazani: le~iani podaci (tlak i temperatura) (tablice 7, 17, 23), sastavi rekombiniranog le~ianog fluida (tablice 8, 18, 24), podaci separator testa (tablice 9, 19, 24), eksperimentalno odreeni tlakovi zasienja pri razli itim temperaturama (tablice 10, 26) podaci dobiveni testom ekspanzije pri stalnom sastavu (tlakovi zasienja pri razli itim temperaturama, relativni volumeni, udio retrogradnog kondenzata, Z faktor plina) (tablice 11, 20, 27), podaci diferencijalnog otparavanja pri stalnom volumenu za plinsko kondenzatne sustave (udio retrogradnog kondenzata, Z faktor plina) (tablica 16), podaci diferencijalnog otparavanja za naftne fluide (plinski faktor, volumni faktor nafte, gustoa nafte) (tablice 21, 28) te viskoznosti (tablica 22) za naftne fluide. Eksperimentalno odreenim PVT podacima iz prethodnih tablica provjerena je konzistentnost na sljedei na in: u injen je prora un masenog uravnote~enja provedenih separatorskih testova (poglavlje 4.1.2.1), u injen je prora un materijalnog uravnote~enja provedenih laboratorijskih ispitivanja (poglavlje 4.1.2.2 i 4.1.2.3), grafi ke provjere analiza sastava tijekom testova otparavanja (4.1.2.4). Maseno uravnote~enje separator testa Koristei kao temelj 1 m3 nafte pri standardnim uvjetima, uz poznavanje eksperimentalno odreenih parametara gustoe nafte, proizvodnog plinskog faktora i relativne gustoe plina pri standardnim uvjetima, mogue je izra unati ukupnu masu proizvedenog plina i nafte iz tog volumena. Analogno tome, uz poznavanje gustoe i volumnog faktora nafte pri le~ianim uvjetima mogue je izra unati ekvivalentnu masu le~iane nafte. Usporeujui dvije izra unate vrijednosti mase analiziranog fluida, ulaznu i izlaznu, utvruje se ravnote~a ili eventualni gubitak mase tijekom provedbe PVT analize. Prora un masenog uravnote~enja izveden je preko sljedeih jednad~bi: volumni faktor nafte pri le~ianim uvjetima:  EMBED Equation.3  (4-1) gdje se kao temelj uzima Vosc=1m3 masa nafte pri le~ianim uvjetima (podaci pri le~ianim uvjetima iz CCE):  EMBED Equation.3  (4-2)  EMBED Equation.3 (kg) masa nafte pri standardnim uvjetima:  EMBED Equation.3  (4-3)  EMBED Equation.3 (kg) masa pripadajueg plina pri standardnim uvjetima:  EMBED Equation.3  (4-4)  EMBED Equation.3 (kg) Ulazni podaci koriateni u ra unu masenog uravnote~enja dobiveni su eksperimentalnim ispitivanjima tijekom provedbe separator testa uzorka C-3-1. Razlika izmeu mase le~ianog i proizvedenog fluida pri standardnim uvjetima od 1,035% ato je prihvatljivo (granica je 2%, Whitson, 2012). Prora un masenog uravnote~enja separator testa prikazan na ovom primjeru proveden je i za ostale uzorke. Materijalno uravnote~enje testa diferencijalnog otparavanja Nakon provedbe testa diferencijalnog otparavanja nafte, potrebno je izvraiti kontrolu eksperimentalno odreenih podataka metodom materijalnog uravnote~enja. Za prora un koristimo sljedee jednad~be:  EMBED Equation.3  (4-5) gdje su:  EMBED Equation.3  gustoa nafte (kg/m3)  EMBED Equation.3  relativna gustoa rezidualne nafte (zadnji korak otparavanja, pri 15C, 1bar) GOR plinski faktor (m3/m3) Bo volumni faktor nafte (m3/m3)  EMBED Equation.3  (4-6) gdje su:  EMBED Equation.3  molarni volumen plina (m3/mol)  EMBED Equation.3  koli ina izdvojenog plina (mol) Vor volumen rezidualne nafte (m3) Podatke dobivene prora unom materijalnog uravnote~enja usporeujemo s eksperimentalno odreenima (prilog I, tablica 28). Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 2. Prora un materijalnog uravnote~enja promatranog uzorka tijekom testa diferencijalnog otparavanja p (bar)Bo (m3/m3)GOR (m3/m3)ggDGOR (m3/m3)mg (g)goro (kg/m3)D (%)0,01,0000-----839,1-0,01,00320,000,00000,000,00000,8364836,4-0,00320,01,155323,781,421423,861,63860,7555760,60,71840,01,196737,280,973913,501,60530,7481747,4-0,15170,01,247355,440,850818,161,57350,7329731,9-0,129100,01,295973,680,784618,241,69610,7189717,7-0,120130,1,342192,550,773418,871,43730,7036706,10,340158,91,3991112,040,764219,493,63430,6908690,1-0,112 Prora un materijalnog uravnote~enja testa diferencijalnog otparavanja prikazan je na uzorku C-3-1. Isti postupak proveden je i za ostale uzorke naftnih fluida. Materijalno uravnote~enje testa otparavanja pri stalnom volumenu Prilikom materijalnog uravnote~enja testa otparavanja pri stalnom volumenu usporeene su koli ine tvari rekombiniranog le~ianog plinsko kondenzatnog fluida i zbroj koli ina tvari pri svakom koraku otparavanja. Za prora un sje koriatena sljedea jednad~ba:  EMBED Equation.3  (4-7) gdje su:  EMBED Equation.3  koli ina tvari (kmol)  EMBED Equation.3  molarna masa tvari (kg/kmol)  EMBED Equation.3  masa tvari (kg) Za tekue uzorke eksperimentalno odreene vrijednosti su masa i molarna masa. Za plinske uzorke molarna masa i gustoa plina ra unaju se iz eksperimentalno odreenog sastava u skladu s normom HRN EN ISO 6976, a volumen plina je direktan rezultat o itan tijekom provedbe testa. Prora un materijalnog uravnote~enja testa otparavanja pri stalnom volumenu izvraen je za sve plinsko kondenzatne fluide. Provjere analiza sastava tijekom testova otparavanja Nakon testova diferencijal provedena je njihova kvaliteta na sljedei na in: grafi ki su prikazani komponentni sastavi proizvedenog plina (yi) na logaritamskoj skali u odnosu na tlak, odnosno korak otparavanja (slika 4-16), provjereni su dvofazni Z faktori kod plinskih kondenzata (slika 4-17) Dvofazni Z faktor ra una se u skladu s pretpostavkom da se plinsko kondenzatni sustav ponaaa tijekom proizvodnje kao suhi plin te da je tlak le~iata jednak tlaku rosiata. Ra una se prema formuli 4-8:  EMBED Equation.3  (4-8) gdje su:  EMBED Equation.3  Z faktor pri tlaku rosiata  EMBED Equation.3  kumulativna koli ina proizvedenog fluida grafi ki su prikazani komponentni sastavi tekue faze (xi) na logaritamskoj skali u odnosu na tlak (slika 4-18), grafi ki su prikazani K omjeri izra unati tijekom provedbe prora una materijalnog uravnote~enja na logaritamskoj skali u odnosu na tlak (slika 4-19).  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 16. Grafi ki prikaz komponentnog sastava plinova proizvedenih tijekom otparavanja pri stalnom volumenu za uzorak A-2-9  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 17. Grafi ki prikaz dvofaznog Z faktora tijekom otparavanja pri stalnom volumenu za uzorak A-2-9  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 18. Grafi ki prikaz komponentnog sastava tekue faze (xi) na logaritamskoj skali u odnosu na tlak otparavanja za uzorak A-2-9  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 19. Grafi ki prikaz K omjera na logaritamskoj skali u odnosu na tlak otparavanja za uzorak A-2-9 Podeaavanje parametara jednad~bi stanja na izabrane uzorke Poslije kontrole PVT podataka pristupilo se podeaavanju parametara jednad~be stanja. Obzirom da je u radu obraeno nekoliko razli itih problema koji utje u na postupak termodinami ke karakterizacije le~ianih fluida jednad~bom stanja, postupci podeaavanja parametara jednad~be stanja podijeljeni su u tri odvojena dijela: 1. U poglavlju 4.1.3.1 dan je opis postupka podeaavanja parametara jednad~be stanja po koracima. Obraivao se uzorak nafte C-3-1 te je dana usporedba rezultata s obzirom na tijek podeaavanja jednad~be stanja. 2. U poglavlju 4.1.3.2 prikazana je usporedba rezultata triju jednad~bi stanja. Prva jednad~ba stanja podeaena je prema rezultatima laboratorijskih ispitivanja plinskog kondenzata (uzorak A-2-9) i nafte (uzorak A-2-17) iz istog le~iata u kojem je izra~en gradijent sastava. Druga i trea jednad~ba podeaene su na rezultate ispitivanja pojedina nih uzoraka iz tog le~iata. Dakle, druga jednad~ba podeaena je na uzorak A-2-17, a trea na uzorak A-2-9. 3. U poglavlju 4.1.3.3 prikazana je usporedba rezultata reproduciranih PVT testova jednad~bama stanja podeaenih na rezultate ispitivanja pri razli itim temperaturama od le~iane temperature. Postupak podeaavanja parametara i provjera kvalitete jednad~be stanja na jednom uzorku le~ianog fluida Postupak podeaavanja parametara jednad~be stanja na jednom uzorku proveden je na uzorku C-3-1. C7+ frakcija uzorka je modificiranom Whitsonovom metodom podijeljena u pet pseudo komponenti. Koriatena je Peng Robinsonova jednad~ba stanja, koju je mogue primijeniti na veini le~ianih ugljikovodi nih fluida. Postupak podeaavanja parametara jednad~be stanja proveo se u devet koraka kako je navedeno u tablici 4-3. Postupak je generaliziran na osnovu obrade velikog broja uzoraka nafte, plinskog kondenzata i mokrog plina. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 3. Pregled postupka podeaavanja parametara jednad~be stanja po koracima Korak podeaavanja/ Ime datotekeOpis postupkaKorak br. 1 Ver_0Unesen sastav fluida. Napravljena podjela C7+ frakcije (Whitsonova kvadratura na 5 pseudokomponenti u MS Excelu). Odreena molarna masa, relativna gustoa i temperatura vreliata za svaku PS. Uneseni binarni interakcijski parametri istih komponenata preporu eni za Peng Robinsonovu jednad~bu stanja (tablica 2-7).Korak br. 2 Ver_1Podeaeni binarni interakcijski parametri za sve pseudokomponente odreeni tako da pribli~e tlakove zasienja eksperimentalnim.Korak br. 3 Ver_2Napravljena regresija binarnog interakcijskog parametra zadnje pseudokomponente prema eksperimentalno odreenim vrijednostima tlakova zasienja.Korak br. 4 Ver_3Napravljena regresija kriti nih temperatura i tlakova pseudokomponenata prema eksperimentalno odreenim tlakovima zasienja.Korak br. 5 Ver_4Napravljena regresija kriti nih temperatura, kriti nih tlakova, acentri nih faktora i volumnih pomaka pseudokomponenata prema eksperimentalno odreenim podacima o tlakovima zasienja, separatorskom proizvodnom plinskom faktoru i gustoi otplinjene nafte.Korak br. 6 Ver_5Napravljena regresija kriti nih temperatura, kriti nih tlakova, acentri nih faktora i volumnih pomaka pseudokomponenata prema eksperimentalno odreenim podacima o tlakovima zasienja, separatorskim proizvodnim plinskim faktorima, gustoi otplinjene nafte i proizvodnim plinskim faktorima tijekom testa diferencijalnog otparavanja.Korak br. 7 Ver_6Napravljena regresija kriti nih temperatura, kriti nih tlakova, acentri nih faktora i volumnih pomaka pseudokomponenata prema eksperimentalno odreenim podacima o tlakovima zasienja, separatorskim proizvodnim plinskim faktorima, gustoi otplinjene nafte, proizvodnim plinskim faktorima i gustoama nafte tijekom testa diferencijalnog otparavanja.Korak br. 8 Ver_7Napravljena regresija kriti nih temperatura, kriti nih tlakova, acentri nih faktora i volumnih pomaka pseudokomponenata prema eksperimentalno odreenim podacima o tlakovima zasienja, separatorskim proizvodnim plinskim faktorima, gustoi otplinjene nafte, proizvodnim plinskim faktorima i gustoama nafte tijekom testa diferencijalnog otparavanja s veim brojem uklju enih eksperimentalnih podataka i veim ponderacijskim faktorima na gustoe nafte.Korak br. 9 Ver_FVNapravljena regresija kriti nih temperatura, kriti nih tlakova, acentri nih faktora i volumnih pomaka pseudokomponenata prema eksperimentalno odreenim podacima o tlakovima zasienja, separatorskim plinskim faktorima iz oba stupnja separacije, gustoi otplinjene nafte, proizvodnim plinskim faktorima i gustoama nafte tijekom testa diferencijalnog otparavanja s veim brojem uklju enih eksperimentalnih podataka i veim ponderacijskim faktorima na gustoe nafte. Podeaeni parametri jednad~be stanja iz zadnjeg koraka regresije (korak br. 9) dani su u tablici 4-4, zajedno s pripadajuim binarnim interakcijskim parametrima u tablici 4-5. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 4. Parametri kona ne (korak br. 9) podeaene jednad~be stanja  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 5. Binarni interakcijski parametri  Slikama od 4-20 do 4-27 grafi ki je prikazan tijek podeaavanja pojedinih testova. Uo ljivo je vrlo dobro slaganje eksperimentalnih i izra unatih podataka u zavranoj verziji ato ukazuje na kvalitetno provedene PVT analize i dobro odreenu jednad~bu stanja.  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 20. Prikaz faznih dijagrama svih verzija jednad~be stanja. Puna linija prikazuje jednad~bom stanja izra unate granice dvofaznog podru ja dok su eksperimentalni podaci prikazani zelenim oznakama. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 6. Usporedba rezultata separatorskog testa po koracima Ver_0Ver_1Ver_2Ver_3Ver_4Ver_5Ver_6Ver_7Ver_FVExp.ParametarIzra unate vrijednostiGOR153,7759,8960,0459,6661,9358,4759,2660,1360,9563,89GOR240,6333,0932,8933,4734,7532,2232,1132,3532,7835,46r1776,7783,25783,42776,48802,71768,62774,95783,97793,5790,84r2825,65824,67824,64817,46848,08806,99812,73822,83833,87832,69Odstupanja= EMBED Equation.3 GOR1-10,12-4,00-3,85-4,23-1,96-5,42-4,63-3,76-2,94GOR25,17-2,37-2,57-1,99-0,71-3,24-3,35-3,11-2,68r1-14,14-7,59-7,42-14,3611,87-22,22-15,89-6,872,66r2-7,04-8,02-8,05-15,2315,39-25,70-19,96-9,861,18Rezidualna odstupanja EMBED Equation.3  EMBED Equation.3 GOR1-15,84-6,26-6,03-6,62-3,07-8,48-7,25-5,89-4,603,61210,1769GOR214,58-6,68-7,25-5,61-2,00-9,14-9,45-8,77-7,567,55960,0469r1-1,79-0,96-0,94-1,821,50-2,81-2,01-0,870,341,30526,0589r2-0,85-0,96-0,97-1,831,85-3,09-2,40-1,180,141,43445,8053 EMBED Equation.3 149,7666,4065,07235,22198,13613,27343,6976,215,62 EMBED Equation.3 1,45810,97090,96111,82731,67702,95052,20881,04010,2824 GOR1 proizvodni plinski faktor iz prvog stupnja separacije GOR2 plinski faktor iz drugog stupnja separacije r1 gustoa nafte iz prvog stupnja separacije r2 gustoa otplinjene nafte nakon drugog stupnja separacije  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 21. Grafi ki prikaz rezultata separator testa po koracima - proizvodni plinski faktor  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 22. Grafi ki prikaz rezultata separator testa po koracima - gustoa tekue faze  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 23. Grafi ka usporedba rezultata testa ekspanzije pri stalnom sastavu - volumni faktor nafte  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 24. Grafi ka usporedba rezultata testa ekspanzije pri stalnom sastavu - relativni volumen  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 25. Grafi ka usporedba proizvodnog plinskog faktora tijekom testa diferencijalnog otparavanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 26. Grafi ka usporedba gustoe nafte tijekom testa diferencijalnog otparavanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 27. Grafi ka usporedba volumnog faktora nafte tijekom testa diferencijalnog otparavanja Usporedba rezultata jednad~be stanja podeaene na viae uzoraka s rezultatima jednad~bi stanja podeaenih na pojedina nim uzorcima To no odreena jednad~ba stanja koristi se za modeliranje razrade le~iata, prora une protoka fluida te za projektiranje procesa proizvodnje. Zato je nu~no razviti jedinstvenu jednad~bu stanja koja to no opisuje ponaaanje fluida u cijelom le~iatu. U svrhu dokazivanja mogunosti podeaavanja jedinstvene jednad~be stanja za cijelo le~iate u injeno je sljedee: podeaena je jedinstvena jednad~ba stanja za uzorak plinskog kondenzata (uzorak A-2-9) i za uzorak nafte (uzorak A-2-17) iz istog le~iata (JS 1), podeaena je jednad~ba stanja samo na uzorak plinskog kondenzata (uzorak A-2-9) (JS 2), podeaena je jednad~ba stanja samo na uzorak nafte (uzorak A-2-17) (JS 3), usporeeni su rezultati pojedinih testova reproducirani dobivenim jednad~bama stanja s eksperimentalnim podacima. Usporedba rezultata grafi ki je prikazana na slikama od 4-28 do 4-37. Uo ljivo je bolje slaganje eksperimentalnih podataka iz ispitivanja provedenih na oba uzorka s podacima reproduciranim jedinstvenom jednad~bom stanja od onih podeaenih na pojedina ne uzorke. Podeaavanje parametara Peng Robinsonove jednad~be stanja za sve tri jednad~be provodilo se na isti na in. C7+ frakcije uzoraka podijeljene su modificiranom Whitsonovom metodom u pet pseudo komponenata. Regresija se vraila promjenom binarnih interakcijskih parametara, kriti ne temperature i tlaka, acentri nih faktora i volumnih pomaka pseudo komponenata. Podeaeni parametri jednad~bi stanja dani su u tablicama 4-7 (JS 1), 4-9 (JS 2), 4-11 (JS 3) zajedno s pripadajuim binarnim interakcijskim parametrima u tablicama 4-8, 4-10 i 4-12. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 7. Parametri jednad~be stanja JS 1  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 8. Binarni interakcijski parametri za JS 1  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 9. Parametri jednad~be stanja JS 2  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 10. Binarni interakcijski parametri za JS 2  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 11. Parametri jednad~be stanja JS 3  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 12. Binarni interakcijski parametri za JS 3     Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 28. Grafi ki prikaz faznih krivulja izra unatih s tri jednad~be stanja Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 13. Usporedba rezultata separator testa Uzorak A-2-17Uzorak A-2-9JS 1JS 2JS 3expJS 1JS 2JS 3expGOR 1182,10203,49183,43186,342980,7429323135,642950,44GOR 214,6318,4515,5317,6139,7442,6638,9544,53r 1787,96879,31796,29796,85768,91725,33812,33725,36r 2804,37907,4814,54815,17803,59759,3848,95755,23  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 29. Grafi ki prikaz relativnih volumena plinskog kondenzata tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 30. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 31. Grafi ki prikaz relativnih volumena nafte tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 32. Grafi ki prikaz volumnih faktora nafte tijekom testa ekspanzije pri stalnom sastavu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 33. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 34. Grafi ki prikaz Z faktora plina tijekom testa otparavanja pri stalnom volumenu s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 35. Grafi ki prikaz volumnih faktora nafte tijekom testa diferencijalnog otparavanja s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 36. Grafi ki prikaz proizvodnog plinskog faktora tijekom testa diferencijalnog otparavanja s tri jednad~be stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 37. Grafi ki prikaz gustoe nafte tijekom testa diferencijalnog otparavanja sa tri jednad~be stanja U svrhu validacije jednad~be stanja za cijelo le~iate napravljena je provjera prema kri~noj validaciji. Kod postupka kri~ne validacije izdvaja se jedan ili viae uzoraka iz kalibracijskog skupa i koristi za provjeru modela. Analogno tome, podeaenom jednad~bom stanja na uzorke A-2-9 i A-2-17 (JS 1) reproducirani su pojedini PVT testovi za ostale uzorke iz le~iata. Rezultati reproduciranih i eksperimentalnih vrijednosti za veinu uzoraka promatranog le~iata A bili su u granicama eksperimentalne pogreake. Uzorak A-1-2 nije zadovoljio kriterije postavljene granicama eksperimentalne pogreake. Za njega je ustanovljeno da nije bila dobra stabilnost za vrijeme uzorkovanja na ato je ukazala HCH/Standing korelacija (evidentan gubitak srednje teakih komponenti  najvjerojatnije propuatanje boce s uzorkom). Primjeri provedene provjere grafi ki su prikazani kroz najva~nije parametre testova otparavanja (slika 4-38 za plinski kondenzat i slika 4-39 na naftu) te tlakova zasienja (slika 4-40).  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 38. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu za uzorak A-6-2 (plinski kondenzat)  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 39. Grafi ki prikaz plinskog faktora tijekom testa diferencijalnog otparavanja za uzorak A-2-13 (nafta)  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 40. Fazni dijagrami reproducirani jedinstvenom jednad~bom stanja Na grafi kim prikazima molarne mase u odnosu na relativnu gustou C7+ frakcije (slika 4-1) i Watsonovog karakterizacijskog faktora (slika 4-2) uo ava se podudarnost podataka iz uzoraka polja E s uzorcima polja A. U skladu s Austad et al. (1983) radom napravljena je provjera uklapanja uzorka E-2-3 s podeaenom jednad~bom stanja polja A (JS 1). Podjela C7+ frakcije uzorka E-2-3 izvraena je u skladu s njezinom proairenom kromatografskom analizom na pet pseudo komponenata kako bi se sastav mogao uvrstiti u jednad~bu stanja JS 1. Dobiveni rezultati pokazali su jako dobro uklapanje na postojeu jednad~bu stanja za polje A te su prikazani na slikama 4-41 i 4-42 za najva~nije parametre (tlak zasienja i krivulju retrogradne kondenzacije tijekom otparavanja pri stalnom volumenu).  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 41. Fazni dijagrami reproducirani jedinstvenom jednad~bom stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 42. Udio retrogradne kondenzacije tijekom testa otparavanja pri stalnom volumenu reproduciran jedinstvenom jednad~bom stanja Rezultati termodinami kih ispitivanja provedenih pri temperaturama razli itim od le~iane temperature Zbog problema karakterizacije le~ianih ugljikovodi nih fluida u uvjetima blizu kriti ne to ke ili pri izrazito visokim temperaturama, pristupilo se razvoju procedure za termodinami ku karakterizaciju pri temperaturama razli itim od le~iane temperature. U tu svrhu, viaekratno se proveo ve ranije u ovom poglavlju prezentiran generalizirani postupak podeaavanja jednad~be stanja. Za izabrani uzorak u injeno je sljedee: podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri temperaturi 35C (JS 35), podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri temperaturi 55C (JS 55), podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri temperaturi 75C (JS 75), podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri temperaturi 95C (JS 95), podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri temperaturi le~iata od 119C (JS 119), podesila se jednad~ba stanja na eksperimentalne podatke ispitivanja provedenih pri svim temperaturama (JS SVE), napravljena je statisti ka obrada podataka promatrajui kvalitete podeaenih jednad~bi stanja usporedbom zbroja apsolutnih relativnih odstupanja te metodom zbroja kvadrata ponderiranih rezidualnih odstupanja. Tablica 29 u prilogu II prikazuje izra unate tlakove zasienja i gustoe fluida pri tim tlakovima za airoki raspon temperatura od 20 do 200C. Slike 4-43 i 4-44 daju grafi ke prikaze istih podataka. Na oba grafa prikazana su odstupanja od 2% od eksperimentalnih vrijednosti za tlak zasienja, odnosno od mediana za gustou fluida. Mogue je zaklju iti da sve jednad~be stanja, osim JS 35, zadovoljavajue reproduciraju tlakove zasienja od najni~e temperature do 140C. Pri temperaturama viaim od 140C dolazi do prevelikog rasipanja rezultata te nije mogue dati jednozna no pozitivnu ocjenu reproduciranja tlakova zasienja. Sli no tome, gustoe fluida izvrsno se reproduciraju svim jednad~bama stanja (osim JS 35) sve do temperature od 150C, iznad koje dolazi do zna ajnijeg rasipanja.  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 43. Grafi ki prikaz tlakova zasienja u rasponu temperatura od 20C do 200C reproduciranih razli itim jednad~bama stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 44. Grafi ki prikaz gustoa pri tlakovima zasienja u rasponu temperatura od 20C do 200C reproduciranih razli itim jednad~bama stanja Razmatrajui temperaturno podru je obuhvaeno izvraenim PVT ispitivanjima u injena je obrada podataka o tlakovima zasienja pri 35C, 55C, 75C, 95C i 119C. Tablica 4-14 sadr~i podatke s tlakovima zasienja, a tablica 4-15 prikazuje usporedbu izra unatih vrijednosti s eksperimentalno odreenim tlakovima zasienja. Jednad~ba stanja JS 35 ima najvee prosje no apsolutno odstupanje u odnosu na druge jednad~be. Pa ipak ak i ona ima relativna odstupanja manja od 2% osim za najviau temperaturu. Grafi ki prikaz relativnih odstupanja prikazan je na slici 4-45. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 14. Izra unati i eksperimentalno odreeni tlakovi zasienja TTlak zasienja (bar)(C)JS 35JS 55JS 75JS 95JS 119JS SVEJS 1EXP119,0362,5352,0348,7350,5348,6352,4349,7352,395,0376,9370,5369,1371,1369,8372,0371,5371,875,0386,6381,5381,1383,3382,3383,4384,7380,455,0392,5388,0388,4390,8390,2390,1393,1388,635,0394,3389,9391,1393,8393,5392,1397,0395,5 Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 15. Odstupanja tlakova zasienja izra unatih pojedinim jednad~bama stanja u odnosu na eksperimentalno odreene vrijednosti JST (C)Odstupanje (bar)Relativno odstupanje (%)Apsolutno rel. odstupanje (%)Prosje no apsolutno rel. odstupanje (%)JS 35119,010,242,912,911,4595,05,141,381,3875,06,211,631,6355,03,931,011,0135,0-1,25-0,320,32JS 55119,0-0,35-0,100,100,4695,0-1,25-0,340,3475,01,120,290,2955,0-0,60-0,150,1535,0-5,60-1,411,41JS 75119,0-3,65-1,041,040,6295,0-2,71-0,730,7375,00,700,180,1855,0-0,18-0,050,0535,0-4,44-1,121,12JS 95119,0-1,79-0,510,510,4995,0-0,69-0,190,1975,02,890,760,7655,02,240,580,5835,0-1,71-0,430,43JS 119119,0-3,73-1,061,060,6195,0-2,03-0,550,5575,01,950,510,5155,01,630,420,4235,0-2,04-0,520,52JS SVE119,00,080,020,020,4295,00,240,060,0675,03,000,790,7955,01,470,380,3835,0-3,44-0,870,87JS 1119,0-2,56-0,730,730,6995,0-0,25-0,070,0775,04,251,121,1255,04,511,161,1635,01,540,390,39  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 45. Grafi ki prikaz relativnih odstupanja izra unatih tlakova zasienja u odnosu na eksperimentalno odreene vrijednosti tlaka zasienja Za daljnju validaciju metode termodinami ke karakterizacije ugljikovodika eksperimentalnim podacima pri temperaturama razli itim od temperature le~iata napravljena je usporedba podataka testa ekspanzije pri stalnom sastavu pri najni~oj odabranoj i eksperimentalno ispitanoj temperaturi od 35C. U prilogu II nalaze se tablice u kojima su prikazani podaci o udjelu retrogradnog kondenzata, relativnom volumenu i Z faktoru plina reproducirani jednad~bama stanja JS 35 (tablica 30), JS 55 (tablica 31), JS 75 (tablica 32), JS 95 (tablica 33), JS 119 (tablica 34) i JS SVE (tablica 35). Grafi ka usporedba izra unatih i eksperimentalnih podataka dana je na slikama 4-46 (udio retrogradnog kondenzata), 4-47 (relativni volumen) i 4-48 (Z faktor plina). Za posljednja dva parametra uo ljivo je vrlo malo rasipanje rezultata izra unatih svim jednad~bama stanja (unutar 2% za relativni volumen te unutar 1% za Z faktor plina). Nasuprot tome, udio retrogradnog kondenzata znatno odstupa ovisno o koriatenoj jednad~bi stanja. Mogue je zaklju iti da se jednad~bom stanja koja je podeaena na eksperimentalne podatke pri najviaoj temperaturi (119C) ne reproducira zadovoljavajue retrogradnu kondenzaciju na najni~oj temperaturi (35) jer su odstupanja viaa od 10%.  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 46. Grafi ki prikaz udjela retrogradnog kondenzata tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 47. Grafi ki prikaz relativnog volumena tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 48. Grafi ki prikaz Z faktora plina tijekom CCE testa pri 35C reproduciranog razli itim jednad~bama stanja Nadalje, napravljena je usporedba podataka testa ekspanzije pri stalnom sastavu pri najviaoj odabranoj i eksperimentalno ispitanoj temperaturi le~iata (119C). U tablicama su prikazani podaci o udjelu retrogradnog kondenzata, relativnom volumenu i Z faktoru plina reproducirani jednad~bama stanja JS 35 (32), JS 55 (tablica 33), JS 75 (tablica 34), JS 95 (tablica 35), JS 119 (tablica 36) i JS SVE (tablica 37). Grafi ka usporedba izra unatih i eksperimentalnih podataka dana je na slikama 4-49 (udio retrogradnog kondenzata), 4-50 (relativni volumen) i 4-51 (Z faktor plina). Isto kao pri najni~oj temperaturi, uo ljivo je vrlo malo rasipanje rezultata izra unatih svim jednad~bama stanja za relativni volumen (unutar 2%) te Z faktor (unutar 1%). Udio retrogradnog kondenzata jednako znatno odstupa ovisno o koriatenoj jednad~bi stanja. Analogno najni~oj temperaturi, jednad~bom stanja koja je podeaena na eksperimentalne podatke pri najni~oj temperaturi (35C) ne reproducira se zadovoljavajue retrogradnu kondenzaciju na najviaoj temperaturi (119).  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 49. Grafi ki prikaz udjela retrogradnog kondenzata tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 50. Grafi ki prikaz relativnog volumena tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 51. Grafi ki prikaz Z faktora plina tijekom CCE testa pri 119C reproduciranog razli itim jednad~bama stanja S ciljem provjere uspjeanosti pojedine regresije napravljena je statisti ka obrada podataka udjela retrogradnog kondenzata pri najni~oj (35C) i najviaoj temperaturi (119C) budui da se prethodnom analizom pokazalo kako taj parametar najviae varira ovisno o jednad~bi stanja koja se koristi. Rezidualna odstupanja izra unatih vrijednosti od eksperimentalno odreenih izra unata su u skladu s jednad~bom 2-94, dok je zbroj ponderiranih rezidualnih odstupanja izra unat po jednad~bi 2-96. Izra unati ponderacijski (te~inski) faktori mali su broj uslijed velikog standardnog odstupanja reproduciranih vrijednosti (jednad~ba 2-95). Provedena statisti ka obrada potvrdila je ve uo enu pravilnost vee pogreake predvianja udjela retrogradnog kondenzata s poveanjem razlike u temperaturi. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 16. Statisti ka obrada udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu pri 35C reproduciranog pojedinim jednad~bama stanja  Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 17. Statisti ka obrada udjela retrogradnog kondenzata tijekom testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi (119C) reproduciranog pojedinim jednad~bama stanja  Najva~niji parametar termodinami ke karakterizacije plinsko kondenzatnih fluida sa stajaliata le~ianog in~enjeringa je retrogradna kondenzacija odreena tijekom testa otparavanja pri stalnom volumenu. Taj podatak: govori o koli ini kondenzata koja e zaostati u le~iatu, upozorava na mogunost blokade pribuaotinske zone kondenzatom u uskoj je vezi sa tzv. tekuim komponentama (C5+) koje se proizvode na povraini (Whitson, 2012). U tablici 4-18 te na slici 4-52 prikazani su udjeli retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu reproducirani pojedinim jednad~bama stanja te eksperimentalni podaci. Podaci su dodatno statisti ki obraeni, ato je prikazano u tablicama 4-19 i 4-20. Primjetan je trend boljeg slaganja reproduciranih (izra unatih jednad~bom stanja) podataka s eksperimentalnim ato je manja razlika u temperaturi (u odnosu na le~ianu temperaturu pri kojoj je raen test otparavanja). Pa ipak mo~e se zaklju iti da sve jednad~be stanja, osim one na najni~oj temperaturi (35C), daju zadovoljavajue rezultate jer su u granicama eksperimentalne pogreake. Takoer je evidentno da jednad~ba stanja iji su se parametri podeaavali na eksperimentalne podatke pri svim temperaturama daje najbolje rjeaenje. Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 18. Volumeni retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu provedenog pri 119C i reproduciranog pojedinim jednad~bama stanja T (C)p (bar)Vliq (%)JS 35JS 55JS 75JS 95JS 119JS SVEEXP119,0352,30,500,000,000,000,000,000,00119,0300,02,241,911,671,661,601,481,49119,0250,03,143,083,063,093,103,243,15119,0200,03,733,753,953,994,054,244,16119,0150,04,074,104,314,384,444,644,58119,0100,04,084,104,284,254,404,604,61119,060,03,853,864,024,004,144,314,42 Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 19. Relativna odstupanja volumena retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu provedenog pri 119C od reproduciranog pojedinim jednad~bama stanja TpRelativno odstupanje (%)(C)(bar)JS 35JS 55JS 75JS 95JS 119JS SVE119,0300,050,4028,5012,1311,407,20-0,76119,0250,0-0,35-2,36-2,79-1,90-1,643,00119,0200,0-10,43-9,85-5,01-4,09-2,712,02119,0150,0-11,20-10,57-5,98-4,34-3,041,31119,0100,0-11,40-11,00-7,15-7,72-4,46-0,15119,060,0-12,95-12,66-8,99-9,46-6,35-2,58Zbroj apsolutnih relativnih odstupanja96,7474,9342,0438,9025,399,83Tablica  STYLEREF 1 \s 4 SEQ Tablica \* ARABIC \s 1 20. Statisti ka obrada rezultata testa otparavanja pri stalnom volumenu provedenog pri 119C i reproduciranog pojedinim jednad~bama stanja TpRezidualno odstupanje(w(C)(bar)JS 35JS 55JS 75JS 95JS 119JS SVE119,0300,050,4028,5012,1311,407,20-0,7618,47520,0008119,0250,0-0,35-2,36-2,79-1,90-1,643,002,13020,0148119,0200,0-10,43-9,85-5,01-4,09-2,712,024,65640,0089119,0150,0-11,20-10,57-5,98-4,34-3,041,314,73690,0097119,0100,0-11,40-11,00-7,15-7,72-4,46-0,154,22520,0109119,060,0-12,95-12,66-8,99-9,46-6,35-2,583,92890,0112Zbroj kvadrata rezidualnih odstupanja0,16600,07730,02070,01820,00700,0010  Slika  STYLEREF 1 \s 4 SEQ Slika \* ARABIC \s 1 52. Grafi ki prikaz udjela retrogradnog kondenzata tijekom testa otparavanja pri stalnom volumenu pri 119C i reproduciranog razli itim jednad~bama stanja Procedure termodinami ke karakterizacije le~ianih fluida Preporu ena procedura termodinami ke karakterizacije jednog uzorka Prvenstveno treba rei da se openito ne preporu a podeaavanje parametara jednad~be stanja na podatke laboratorijskih ispitivanja samo jednog uzorka. No meutim, ukoliko ne postoje drugi dostupni podaci ili ako se dostupni podaci doka~u nekvalitetnima, rad u skladu s ovom procedurom je dobar po etak. Na primjer, u po etnoj fazi istra~ivanja nekog novog prostora bitno je ato prije imati smjernice koje e pokazivati u kojom smjeru nastaviti istra~ivanje. U po etnoj fazi istra~ivanja nekog novog prostora bitno je ato prije imati stanovitu karakterizaciju fluida koja predstavlja smjernice za ulaganje i izvedbu u detaljnija istra~ivanja. Ve nakon prve izbuaene buaotine i prvog uzorkovanog fluida mogue je napraviti PVT ispitivanja te na osnovu njihovih rezultata podesiti jednad~bu stanja koja mo~e predvidjeti fazne promjene uzorkovanog fluida u airokom tla no temperaturnom podru ju. Tek kasnije, uzimanjem uzoraka iz viae buaotina, poveava se sigurnost predikcije ponaaanja le~ianih fluida. Uzorkovanje se takoer nastavlja i tijekom proizvodnje, za provjeru i korekciju ranije odreenih svojstava le~iata i fluida u le~iatu. Preporu ena procedura termodinami ke karakterizacije jednog uzorka je sljedea: Izvraiti kontrolu kvalitete (utvrditi reprezentativnost) uzorka: provjera trenda krivulje molni udio u odnosu na jedinstveni uglji ni broj za stabilizirane uzorke nafte, kondenzata ili C7+ frakcije u log-normalnom dijagramu provjera K omjera za ugljikovodi ne komponente Hoffman-Crump-Hocott metodom te usporedba linearnog trenda s vrijednostima Standingove korelacije Izvraiti laboratorijska PVT ispitivanja na uzorku koji je utvren kao reprezentativan: rutinska PVT ispitivanja (utvrivanje tla no-volumnih odnosa i kontaktno otplinjavanje separatorske nafte, kromatografske analize separatorskog plina, plina iz kontaktnog otplinjavanja te stabilizirane nafte, odreivanje gustoe stabilizirane nafte, frakcijska destilacija nafte u svrhu karakterizacije pseudokomponente te prora un sastava ukupnog proizvedenog le~ianog fluida) specijalne analize (test ekspanzije uzorka pri stalnom sastavu, testovi otparavanja - diferencijalno za naftu, pri stalnom volumenu za plinove, separator test, odreivanje viskoznosti i gustoe pri le~ianim uvjetima) Provjeriti kvalitetu izvraenih PVT ispitivanja materijalno i maseno uravnote~enje grafi ke provjere sastava plinskih i tekuih faza provjera K omjera za testove otparavanja Podesiti parametre jednad~be stanja na rezultate PVT ispitivanja izabrati jednad~bu stanja, ovisno o mogunostima koje nudi simulacijski softver koji se koristi upisati sastav proizvedenog fluida (uzorka) i sve PVT laboratorijske podatke koji su kroz provjere iz 3. to ke dokazani kvalitetnima podesiti binarne interakcijske koeficijente - za iste komponente koriste se preporu ene vrijednosti (ovisno o izabranoj jednad~bi stanja), dok se za pseudokomponente podeaavaju dok se ne podese eksperimentalno odreeni tlakovi zasienja vraiti postepenu regresiju u viae koraka mijenjajui kriti na svojstva, acentri ne faktore, parametre volumnog pomaka i omega A i B pseudo komponenata sve dok se ne postigne zadovoljavajue slaganje s eksperimentalnim podacima. Regresija se vrai po koracima uklju ujui sve vei broj eksperimentalnih podataka s obzirom na koje se jednad~ba stanja usklauje, i to redom: tlakove zasienja, podatke separator testa (plinski faktor, gustoa, volumni faktor), podatke iz testa ekspanzije pri stalnom sastavu, podatke iz testova otparavanja. `to je vei broj podataka na koje se podeaava jednad~ba stanja to postoji vea potreba za parametrima koje je mogue regresirati pa ih tako postepeno dodajemo. To radimo redoslijedom kako su prethodno nabrojani od kriti nih svojstava pa do omega A i B. Provjeriti kvalitetu jednad~be stanja provjera integriteta i monotonosti krivulja dobivenih podeaenom jednad~bom stanja grafi ka obrada podataka - usporedbe eksperimentalno odreenih podataka s pripadajuim podacima reproduciranih PVT testova izra unatih podeaenom jednad~bom stanja tijek provjeravanja podeaene jednad~be stanja: fazne krivulje - tlakovi zasienja prora un separatorskih podataka (plinski faktor, gustoa, volumni faktor) prora un testa ekspanzije pri stalnom sastavu nafte: relativni volumeni, volumni faktor nafte, gustoa nafte kondenzati: relativni volumeni, volumen retrogradnog kondenzata, faktor kompresibilnosti testovi otparavanja nafte: diferencijalno otparavanje (plinski faktor, volumni faktor nafte, gustoa nafte) kondenzati: otparavanje pri stalnom volumenu (volumen retrogradnog kondenzata, volumni faktor plina, faktor kompresibilnosti). Preporu ena procedura termodinami ke karakterizacije viae uzoraka Termodinami ku karakterizaciju za le~iate s izra~enim gradijentom sastava kakvo je razmatrano u radu, preporu a se vraiti na sljedei na in: Izbor najboljih uzoraka (provjere to nosti uvjeta i kvalitete separacije, provjere to nosti i broj provedenih eksperimentalnih ispitivanja, reprezentativnost uzorka za promatrano podru je). Uklapanje najmanje dva reprezentativna uzorka istovremeno. Usporedba s PVT ispitivanjima provedenim na drugim uzorcima. Usporedba s proizvodnim podacima i ispitivanjima u buaotini na polju. Sami tijek termodinami ke karakterizacije ne razlikuje se od preporu ene procedure termodinami ke karakterizacije jednog uzorka. Osnovna razlika je ato se podeaavanje parametara jednad~be stanja vrai na viae uzoraka istovremeno. ZAKLJU AK Osnovni ciljevi pri izradi ovog rada bili su: dokazati potrebu za definiranjem jedinstvene jednad~be stanja za le~iata s izra~enim gradijentom sastava te razraditi mogunost podeaavanja parametara jednad~be stanja na eksperimentalne podatke dobivene ispitivanjima pri temperaturama razli itim od temperature le~iata. U radu je posebno te~iate na eksperimentalnim postupcima koji se provode u laboratoriju za termodinami ku karakterizaciju le~ianih ugljikovodi nih fluida, provjeri eksperimentalnih podataka te provjeri podeaene jednad~be stanja. Istra~ivanja provedena tijekom izrade ovog doktorskog rada rezultirala su sljedeim zaklju cima: Jednad~ba stanja koja bi mogla predvidjeti ponaaanje le~ianih ugljikovodi nih fluida u airem rasponu tla no-temperaturnih uvjeta u izrazitoj je ovisnosti o koli ini i kvaliteti provedenih laboratorijskih ispitivanja. U svrhu dokazivanja temeljnih hipoteza ovoga rada, izvraena su brojna eksperimentalna ispitivanja (186 analiza na 40 uzoraka) te ra unalne simulacije PVT testova pri razli itim temperaturama i airokom rasponu tlakova. Uslijed nedostataka dostupnih ra unalnih aplikacija, izraena je interna procedura za razdjeljivanje plus frakcije le~ianog fluida metodom dijeljenja Gaussove kvadrature. Za potrebe predvienog istra~ivanja napravljena je procedura termodinami ke karakterizacije le~ianih fluida koja se temelji na metodama razvijenim i tradicionalno koriatenim u PVT laboratoriju. Poboljaanje procedure o ituje se u integriranom pristupu laboratorijskih ispitivanja i upotrebe eksperimentalno dobivenih PVT podataka u le~ianom in~enjeringu. Preporuka procedure dana je u poglavlju 4.3. Potvrena je temeljna hipoteza istra~ivanja da kubna jednad~ba stanja definirana usklaivanjem parametara na analize uzoraka iz viae buaotina bolje opisuje fluid u cijelom le~iatu nego ato ga opisuje jednad~ba stanja izraena na temelju reprezentativnog uzorka iz jedne buaotine. Potvrena je i druga temeljna hipoteza istra~ivanja da se fazno ponaaanje i volumne promjene le~ianih fluida mogu opisati kubnom jednad~bom stanja usklaenom na PVT podatke dobivene laboratorijskim ispitivanjima pri temperaturama razli itim od le~iane. Time se omoguuje eksperimentalna karakterizacija fluida ije le~iane temperature premaauju maksimalne radne temperature postojee opreme na svjetskom tr~iatu kao i bolju karakterizaciju fluida blizu kriti ne to ke. Provedba PVT testova na temperaturama ni~im od le~iane temperature znatno e smanjiti troakove laboratorijskih analiza. 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(1979): Application of a Generalized Equation of State to Petroleum Reservoir Fluids Advances in Chemistry, Vol. 182, 385-439. Zuo, J.Y. & Zhang, D. (2000): Plus Fraction Characterization and PVT Data Regression for Reservoir Fluids near Critical Conditions, SPE paper No. 64520. PRILOG I Eksperimentalni podaci Tablica  SEQ Tablica \* ARABIC \s 1 1. Proaireni sastavi za C7+ frakcije izabranih uzoraka `ifra uzorkaA-2-9A-2-17A-1-2E-2-3C-3-1SCN xi (mol%)C70,6582,9181,3610,2045,169C80,5663,1980,7820,3675,120C90,4202,4690,5580,3723,668C100,3232,2830,4370,3673,243C110,2181,7070,2850,2892,742C120,1671,4120,2060,2252,355C130,1551,4430,1840,2062,190C140,1241,4320,1410,1482,196C150,1191,4370,1250,1192,036C160,0791,0320,0750,0621,552C170,0670,9990,0640,0431,684C180,0600,9040,0530,0311,442C190,0490,6010,0420,0191,021C200,0300,5530,0230,0070,893C210,0240,5180,0180,0030,800C220,0200,4360,0140,0010,712C230,0150,4140,010,0010,651C240,0110,3580,0070,2040,573C250,0090,3410,0050,3670,561C260,0080,2890,0040,3720,471C270,0060,2610,0030,3670,469C280,0050,2810,0020,2890,437C290,0040,2560,0030,2250,387C30+0,0131,1150,0040,2063,330 Tablica  SEQ Tablica \* ARABIC \s 1 2. Eksperimentalno odreeni sastavi separatorskih fluida za uzorak A-2-9 KomponentaMgxiyi(kg/kmol)(mol%)(mol%)N228,00,200,77CO244,00,832,14C116,013,7990,57C230,12,483,24C344,14,601,66i-C458,10,57041,720,30n-C458,10,59065,410,69i-C572,20,62953,820,21n-C572,20,63595,560,18C684,10,70617,770,14C7+160,600,786853,830,11GOR (m3sc/m3sep)2624,25Tsep (C)19,5psep (bar)30,0 Tablica  SEQ Tablica \* ARABIC \s 1 3. Eksperimentalno odreeni sastavi separatorskih fluida za uzorak A-2-17 KomponentaMgxiyi(kg/kmol)(mol%)(mol%)N228,00,040,39CO244,00,150,86C116,06,0687,17C230,13,166,18C344,15,433,32i-C458,10,57041,540,45n-C458,10,59064,740,89i-C572,20,62952,660,22n-C572,20,63593,120,20C684,10,70615,100,13C7+225,410,841268,000,19GOR (m3sc/m3sep)176,66Tsep (C)23,5psep (bar)14,8 Tablica  SEQ Tablica \* ARABIC \s 1 4. Eksperimentalno odreeni sastavi separatorskih fluida za uzorak C-3-1 KomponentaMgxiyi(kg/kmol)(mol%)(mol%)N228,00,011,44CO244,00,291,13C116,09,3481,38C230,15,669,84C344,17,644,25i-C458,10,57041,580,48n-C458,10,59064,480,84i-C572,20,62952,260,21n-C572,20,63592,570,18C684,10,70613,920,12C7+220,420,852862,260,13GOR (m3sc/m3sep)57,17Tsep (C)34,0psep (bar)30,0 Tablica  SEQ Tablica \* ARABIC \s 1 5. Eksperimentalno odreeni sastavi separatorskih fluida za uzorak E-2-3 KomponentaMgxiyi(kg/kmol)(mol%)(mol%)N228,00,131,27CO244,00,771,44C116,022,8090,15C230,14,043,60C344,15,541,76i-C458,10,57042,140,37n-C458,10,59065,140,63i-C572,20,62954,180,25n-C572,20,63594,080,19C684,10,70618,320,18C7+211,370,825742,870,16GOR (m3sc/m3sep)12163,2Tsep (C)28,5psep (bar)60,0 Tablica  SEQ Tablica \* ARABIC \s 1 6. Eksperimentalno odreeni sastavi separatorskih fluida za uzorak A-1-2 KomponentaMgxiyi(kg/kmol)(mol%)(mol%)N228,00,270,92CO244,00,380,60C116,025,5789,09C230,15,424,52C344,17,022,07i-C458,10,57041,920,32n-C458,10,59065,830,70i-C572,20,62953,270,25n-C572,20,63594,410,27C684,10,70616,010,64C7+211,370,825739,910,63GOR (m3sc/m3sep)1787,3Tsep (C)22,5psep (bar)60,0 Eksperimentalni podaci PVT ispitivanja uzorka plinskog kondenzata A-2-9 Tablica  SEQ Tablica \* ARABIC \s 1 7. Le~iani podaci (tlak i temperatura) Tr (C)119pi (bar)360 Tablica  SEQ Tablica \* ARABIC \s 1 8. Sastav rekombiniranog le~ianog fluida iziN20,737CO22,061C186,231C23,200C31,827C41,335C50,894C60,566C7+3,149MC7+160,60r C7+ (kg/m3)786,76 Tablica  SEQ Tablica \* ARABIC \s 1 9. Podaci separator testa T (C)p (bar)GOR (m3sc/m3sc)Bo (m3/m3sc)ro (kg/m3)19,5302950,441,1243725,3615044,531,0000755,23 Tablica  SEQ Tablica \* ARABIC \s 1 10. Eksperimentalno odreeni tlakovi zasienja T (C)pd (bar)35395,555388,675380,495371,8119352,3 Tablica  SEQ Tablica \* ARABIC \s 1 11. Podaci dobiveni testom ekspanzije pri stalnom sastavu pri le~ianoj temperaturi (relativni volumeni, udio retrogradnog kondenzata, Z faktor plina) T (C)p (bar)Vliq (%)Vrel (m3/m3)Z119400,00,000,92731,0399390,40,000,93981,0287379,70,000,95481,0165370,30,000,96961,006736,000,000,98660,9958352,30,001,00000,9878349,80,071,0042340,50,281,0220319,80,811,0659300,21,331,1153270,22,051,2093239,92,661,3350209,92,911,5032180,22,871,7346149,72,582,0817120,22,162,6006100,31,823,1335 Tablica  SEQ Tablica \* ARABIC \s 1 12. Podaci dobiveni testom ekspanzije pri stalnom sastavu pri 35C (relativni volumeni, udio retrogradnog kondenzata) T (C)p (bar)Vliq (%)Vrel (m3/m3)35400,00,000,9979395,50,001,0000393,10,041,0026389,20,141,0068382,50,331,0134371,20,761,0255352,31,521,0473330,02,651,0756299,54,201,1250270,15,701,1885240,36,821,2774210,37,461,4075179,67,311,6092150,46,741,9183119,95,432,4500100,24,442,9921 Tablica  SEQ Tablica \* ARABIC \s 1 13. Podaci dobiveni testom ekspanzije pri stalnom sastavu pri 55C (relativni volumeni, udio retrogradnog kondenzata) T (C)p (bar)Vliq (%)Vrel (m3/m3)55400,00,000,9924388,60,001,0000385,40,061,0040379,00,211,0093368,20,541,0198359,50,891,0297339,41,801,0571319,52,691,0893300,13,591,1272269,84,921,2025240,95,781,3018210,66,151,4481180,46,021,6648150,35,331,9954120,34,362,5332100,03,573,0914 Tablica  SEQ Tablica \* ARABIC \s 1 14. Podaci dobiveni testom ekspanzije pri stalnom sastavu pri 75C (relativni volumeni, udio retrogradnog kondenzata) T (C)p (bar)Vliq (%)Vrel (m3/m3)75400,00,000,9757389,70,000,9890380,40,001,0000379,60,041,0012369,90,261,0142360,30,561,0275340,21,331,0654320,02,131,1039299,92,901,1487269,73,991,2336240,04,731,3470210,35,041,5044180,44,971,7314150,44,402,0716120,53,592,6054100,32,943,1717 Tablica  SEQ Tablica \* ARABIC \s 1 15. Podaci dobiveni testom ekspanzije pri stalnom sastavu pri 95C (relativni volumeni, udio retrogradnog kondenzata) T (C)p (bar)Vliq (%)Vrel (m3/m3)95400,00,000,9635379,80,000,9887371,80,001,0000367,10,091,0072360,00,241,0184349,70,531,0357340,70,821,0521320,01,531,0944300,02,221,1428270,73,221,2317239,73,811,3576210,24,021,5215180,03,931,7580150,13,502,1031120,92,912,6257100,52,393,1865 Tablica  SEQ Tablica \* ARABIC \s 1 16. Podaci diferencijalnog otparavanja pri stalnom volumenu (udio retrogradnog kondenzata, volumni faktor plina, Z faktor plina) T (C)p (bar)Vliq (%)Bg (m3/m3sc)Z119352,30,000,004050,9906300,01,490,004520,9609250,03,150,005150,9311200,04,160,006350,9035150,04,580,008340,8987100,04,610,012670,900660,04,420,021510,9340 Eksperimentalni podaci PVT ispitivanja uzorka nafte A-2-17 Tablica  SEQ Tablica \* ARABIC \s 1 17. Le~iani podaci (tlak i temperatura) Tr (C)113pi (bar)313,2 Tablica  SEQ Tablica \* ARABIC \s 1 18. Sastav rekombiniranog le~ianog fluida iziN20,256CO20,576C155,192C24,989C34,154C43,288C52,529C62,089C7+26,926MC7+225,41r C7+ (kg/m3)0,8412 Tablica  SEQ Tablica \* ARABIC \s 1 19. Podaci separator testa T (C)p (bar)GOR (m3sc/m3sc)Bo (m3/m3sc)ro (kg/m3)23,514,8186,341,0548796,85150,027,611,0000815,17 Tablica  SEQ Tablica \* ARABIC \s 1 20. Podaci dobiveni testom ekspanzije pri stalnom sastavu (relativni volumeni, volumni faktor nafte) T (C)p (bar)Vrel (m3/m3)Bo (m3/m3sc)113400,00,97641,6941380,00,98011,7005360,00,98481,7086340,00,98881,7156320,00,99471,7258300,00,99981,7348298,21,00001,7351280,01,0209268,01,0367247,51,0669224,01,1131173,51,2711124,01,594698,01,921575,02,414258,03,0731 Tablica  SEQ Tablica \* ARABIC \s 1 21. Podaci dobiveni testom diferencijalnog otparavanja (plinski faktor, volumni faktor nafte, gustoa nafte) T (C)p (bar)GOR (m3sc /m3sc)Bo (m3/m3sc)ro (kg/m3)113298,2233,21,7351602,1250,0180,21,5845629,7200,0136,21,4594657,4150,0100,01,3607682,0100,068,51,2792704,250,038,81,1977729,510,011,31,1075758,90,00,01,0286799,60,0822,4 Tablica  SEQ Tablica \* ARABIC \s 1 22. Eksperimentalno odreena viskoznost nafte T (C)p (bar)m (mPas)1134000,3443500,3343200,3293000,3252900,3232700,3242500,3282300,3372100,353 Eksperimentalni podaci PVT ispitivanja uzorka nafte C-3-1 Tablica  SEQ Tablica \* ARABIC \s 1 23. Le~iani podaci (tlak i temperatura) Tr (C)110pi (bar)288,7 Tablica  SEQ Tablica \* ARABIC \s 1 24. Sastav rekombiniranog le~ianog fluida iziN20,448CO20,550C131,536C26,950C36,592C44,601C53,458C62,751C7+43,115MC7+220,42r C7+ (kg/m3)852,76 Tablica  SEQ Tablica \* ARABIC \s 1 25. Podaci separator testa T (C)p (bar)GOR (m3sc/m3sc)Bo (m3/m3sc)ro (kg/m3)343063,891,1179790,8415045,461,0000832,69 Tablica  SEQ Tablica \* ARABIC \s 1 26. Eksperimentalno odreeni tlakovi zasienja T (C)pb (bar)22,6116,150131,280146,8110158,9 Tablica  SEQ Tablica \* ARABIC \s 1 27. Podaci dobiveni testom ekspanzije pri stalnom sastavu (relativni volumeni, volumni faktor nafte) T (C)p (bar)Vrel (m3/m3)Bo (m3/m3sc)ro (kg/m3)110400,00,95921,3420719,4350,00,96591,3514714,4310,00,97201,3599709,9270,00,97791,3683705,6250,00,98091,3724703,5210,00,98871,3833697,9170,00,99721,3952692,0158,91,00001,3991690,1155,31,0084152,21,0161149,31,0237144,01,0391139,01,0546 Tablica  SEQ Tablica \* ARABIC \s 1 28. Podaci dobiveni testom diferencijalnog otparavanja (plinski faktor, volumni faktor nafte, gustoa nafte) T (C)p (bar)GOR (m3sc /m3sc)Bo (m3/m3sc)ro (kg/m3)110158,9112,01,3991690,113092,61,3421706,110073,71,2959717,77055,41,2473731,94037,31,1967747,42023,81,1553760,600,01,0032 PRILOG II Podaci PVT testova reproduciranih jednad~bama stanja podeaenim pri razli itim temperaturama Tablica  SEQ Tablica \* ARABIC \s 1 29. Rezultati tlakova zasienja i gustoe pri tlaku zasienja reproducirani jednad~bama stanja podeaenim pri razli itim temperaturama Tpsatrpsatpsatrpsat(C)(bar)(kg/m3)(bar)(kg/m3)JS 35JS 5520,0392,8364,5388,4363,338,0394,3344,1389,9342,756,0392,3323,6387,8322,074,0387,0302,9381,9301,092,0378,6282,2372,5279,7110,0368,1261,9359,6258,3128,0357,0242,7343,7236,8146,0345,4224,6326,0215,7164,0332,8207,3307,9195,8182,0318,9190,8289,6177,0200,0303,5174,8270,6159,2Tpsatrpsatpsatrpsat(C)(bar)(kg/m3)(bar)(kg/m3)JS 75JS 9520,0390,1364,1393,1364,838,0391,0343,4393,6344,056,0388,2322,4390,6323,074,0381,6301,1383,8301,892,0371,2279,5373,2280,1110,0357,1257,4359,0258,1128,0339,3235,0341,1235,7146,0318,2212,2319,8212,8164,0294,0189,1295,4189,7182,0267,6166,2268,6166,6200,0241,2144,6241,3144,6Tpsatrpsatpsatrpsat(C)(bar)(kg/m3)(bar)(kg/m3)JS 119JS SVE20,0393,0365,2390,6366,438,0393,3344,3392,1345,956,0389,9323,2389,8325,174,0382,9301,8383,8304,092,0372,0280,0374,0282,5110,0357,3257,7360,5260,7128,0338,9234,9343,4238,5146,0316,9211,7323,2216,0164,0291,3187,8308,0197,2182,0262,0163,4289,8178,1200,0229,2138,4270,9159,8 Tablica  SEQ Tablica \* ARABIC \s 1 30. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS 35 TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,572,94490,811635,0115,85,352,50810,794635,0131,66,052,18790,781935,0147,46,631,94710,773835,0163,27,051,76270,770335,0178,97,291,61910,771435,0194,77,371,50580,776835,0210,57,281,41510,786035,0226,37,041,34150,798735,0242,16,651,28090,814535,0257,96,101,23030,832935,0273,75,411,18770,853635,0289,54,621,15120,876435,0305,33,831,11990,900535,0321,13,111,09260,925535,0336,82,451,06850,951235,0352,61,821,04700,977535,0368,41,161,02781,004335,0384,20,471,01031,031635,0400,00,000,99481,0590Tablica  SEQ Tablica \* ARABIC \s 1 31. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS 55 TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,572,93430,811935,0115,85,362,49940,795035,0131,66,062,18060,782435,0147,46,651,94090,774435,0163,27,091,75720,771135,0178,97,361,61410,772335,0194,77,451,50100,777735,0210,57,351,41040,787035,0226,37,041,33670,799835,0242,16,511,27590,815835,0257,95,791,22520,834635,0273,75,011,18260,855535,0289,54,301,14640,878035,0305,33,651,11530,901635,0321,13,021,08810,926135,0336,82,401,06410,951535,0352,61,751,04260,977735,0368,41,051,02341,004435,0384,20,291,00591,031835,0400,00,000,99091,0590Tablica  SEQ Tablica \* ARABIC \s 1 32. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS 75 TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,562,94290,812535,0115,85,362,50740,795935,0131,66,082,18830,783635,0147,46,681,94830,775935,0163,27,141,76430,772835,0178,97,411,62070,774335,0194,77,431,50690,780035,0210,57,151,41530,789735,0226,36,711,34100,803035,0242,16,261,28020,819035,0257,95,811,22960,837235,0273,75,331,18690,857335,0289,54,811,15030,878935,0305,34,241,11860,901835,0321,13,631,09090,925835,0336,82,951,06640,950835,0352,62,211,04450,976635,0368,41,381,02491,003335,0384,20,441,00721,030735,0400,00,000,99201,0580Tablica  SEQ Tablica \* ARABIC \s 1 33. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS 95 TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,542,94610,811735,0115,85,312,50950,794835,0131,66,002,18950,782335,0147,46,571,94900,774335,0163,26,981,76480,771235,0178,97,181,62120,772635,0194,77,131,50750,778535,0210,56,781,41630,788635,0226,36,311,34250,802335,0242,15,881,28220,818835,0257,95,471,23200,837435,0273,75,031,18950,857735,0289,54,571,15310,879535,0305,34,061,12150,902535,0321,13,501,09380,926535,0336,82,891,06930,951535,0352,62,201,04750,977335,0368,41,441,02781,003935,0384,20,581,01001,031235,0400,00,000,99441,0587Tablica  SEQ Tablica \* ARABIC \s 1 34. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS 119 TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,552,95290,812835,0115,85,342,51640,796335,0131,66,062,19650,784235,0147,46,661,95600,776735,0163,27,081,77130,773935,0178,97,271,62700,775535,0194,77,201,51260,781635,0210,57,011,42130,791535,0226,36,791,34730,804635,0242,16,531,28650,820435,0257,96,221,23560,838335,0273,75,841,19240,858035,0289,55,401,15540,879235,0305,34,871,12320,901835,0321,14,271,09500,925435,0336,83,561,07000,950135,0352,62,751,04780,975735,0368,41,811,02781,002335,0384,20,721,00981,029735,0400,00,000,99421,0573Tablica  SEQ Tablica \* ARABIC \s 1 35. Rezultati testa ekspanzije pri stalnom sastavu pri 35C reproduciranog JS SVE TpVliqVrelZ faktor(C)(bar)(%)35,0100,04,712,96190,815935,0115,85,592,52400,799835,0131,66,422,20280,787735,0147,47,141,96060,780035,0163,27,691,77400,776635,0178,97,901,62730,777335,0194,77,471,50970,782635,0210,57,011,41650,791735,0226,36,621,34170,804235,0242,16,161,28030,819435,0257,95,621,22940,837135,0273,75,031,18640,856835,0289,54,411,14990,878135,0305,33,781,11830,900735,0321,13,141,09080,924335,0336,82,501,06660,948735,0352,61,831,04500,973735,0368,41,141,02560,999235,0384,20,391,00811,025135,0400,00,000,99291,0515Tablica  SEQ Tablica \* ARABIC \s 1 36. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS 35 TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,593,13790,9189119,0115,81,832,70320,9136119,0131,62,052,37710,9102119,0147,42,232,12490,9087119,0163,22,381,92500,9091119,0178,92,481,76350,9113119,0194,72,561,63100,9153119,0210,52,591,52080,9210119,0226,32,591,42800,9283119,0242,12,551,34910,9371119,0257,92,471,28140,9473119,0273,72,351,22270,9587119,0289,52,161,17140,9714119,0305,31,911,12630,9852119,0321,11,561,08631,0002119,0336,81,091,05051,0163119,0352,60,481,01851,0336119,0368,40,000,99021,0517119,0384,20,000,96551,0693119,0400,00,000,94301,0872Tablica  SEQ Tablica \* ARABIC \s 1 37. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS 55 TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,613,08060,9193119,0115,81,862,65400,9141119,0131,62,092,33400,9107119,0147,42,282,08640,9092119,0163,22,431,89010,9096119,0178,92,541,73150,9118119,0194,72,611,60130,9157119,0210,52,641,49290,9213119,0226,32,621,40170,9286119,0242,12,551,32410,9374119,0257,92,421,25740,9477119,0273,72,221,19970,9593119,0289,51,951,14920,9722119,0305,31,581,10470,9863119,0321,11,111,06531,0015119,0336,80,571,03021,0176119,0352,60,000,99881,0345119,0368,40,000,97211,0517119,0384,20,000,94781,0694119,0400,00,000,92581,0873Tablica  SEQ Tablica \* ARABIC \s 1 38. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS 75 TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,703,06570,9205119,0115,81,972,64160,9154119,0131,62,222,32340,9121119,0147,42,432,07710,9107119,0163,22,601,88180,9110119,0178,92,731,72380,9132119,0194,72,801,59400,9170119,0210,52,811,48580,9225119,0226,32,751,39460,9297119,0242,12,601,31700,9384119,0257,92,381,25030,9487119,0273,72,081,19250,9602119,0289,51,741,14210,9730119,0305,31,361,09780,9868119,0321,10,931,05861,0015119,0336,80,431,02371,0171119,0352,60,000,99291,0336119,0368,40,000,96631,0509119,0384,20,000,94231,0685119,0400,00,000,92041,0864Tablica  SEQ Tablica \* ARABIC \s 1 39. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS 95 TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,653,07490,9200119,0115,81,912,64940,9149119,0131,62,152,33030,9117119,0147,42,352,08330,9104119,0163,22,521,88750,9109119,0178,92,651,72920,9131119,0194,72,721,59910,9171119,0210,52,731,49070,9228119,0226,32,671,39930,9301119,0242,12,531,32140,9389119,0257,92,311,25450,9492119,0273,72,041,19660,9609119,0289,51,721,14610,9737119,0305,31,361,10170,9874119,0321,10,951,06241,0021119,0336,80,481,02741,0177119,0352,60,000,99621,0342119,0368,40,000,96951,0514119,0384,20,000,94541,0691119,0400,00,000,92341,0870Tablica  SEQ Tablica \* ARABIC \s 1 40. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS 119 TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,763,06760,9213119,0115,82,042,64350,9163119,0131,62,292,32530,9131119,0147,42,512,07900,9118119,0163,22,691,88360,9122119,0178,92,821,72540,9144119,0194,72,871,59530,9182119,0210,52,861,48690,9238119,0226,32,771,39550,9309119,0242,12,611,31770,9395119,0257,92,411,25090,9495119,0273,72,151,19300,9608119,0289,51,841,14250,9732119,0305,31,471,09810,9866119,0321,11,021,05871,0011119,0336,80,481,02371,0165119,0352,60,000,99271,0330119,0368,40,000,96621,0503119,0384,20,000,94221,0679119,0400,00,000,92031,0859Tablica  SEQ Tablica \* ARABIC \s 1 41. Rezultati testa ekspanzije pri stalnom sastavu pri le~ianoj temperaturi reproduciranog JS SVE TpVliqVrelZ faktor(C)(bar)(%)119,0100,01,873,09650,9212119,0115,82,162,66770,9159119,0131,62,432,34580,9123119,0147,42,652,09650,9104119,0163,22,831,89870,9103119,0178,92,961,73860,9119119,0194,73,041,60710,9152119,0210,53,041,49750,9202119,0226,32,971,40530,9269119,0242,12,801,32670,9352119,0257,92,511,25920,9451119,0273,72,061,20060,9567119,0289,51,581,14970,9694119,0305,31,201,10520,9827119,0321,10,831,06590,9967119,0336,80,441,03091,0113119,0352,60,000,99961,0266119,0368,40,000,97291,0438119,0384,20,000,94881,0615119,0400,00,000,92681,0794 PRILOG III }ivotopis autora Roena sam u 12. srpnja 1976. godine u Zagrebu. Nakon zavraenog osnovnog i srednjeg obrazovanja (V. gimnazija, Zagreb) upisala sam Rudarsko-geoloako-naftni fakultet Sveu iliata u Zagrebu smjer naftno rudarstvo ak. god. 1995/96., te diplomirala 2001. godine na temu  Analiza hermeti nosti sustava CPS III - Molve i stekla zvanje diplomiranog in~enjera naftnog rudarstva. Zaposlena sam od 10.07.2002. godine u INA  Industrija nafte d.d., SD Istra~ivanje i proizvodnja nafte i plina  Naftaplin u Slu~bi laboratorijskih ispitivanja kao naftni in~enjer u Laboratoriju za PVT, EOR i reologiju. Tijekom svog radnog vijeka osim laboratorijskih istra~ivanja i ispitivanja, izrade prora una s interpretacijama dobivenih podataka, izrade izvjeaa i zahtjevnih studija, sudjelovala sam na mnogim znanstveno-stru nim skupovima s radovima, usavraavala se dodatnim stru nim znanjima kroz inozemne i tuzemne te ajeve, sudjelovala u projektima, dobila nagrade za inovacije i dr. Zavraila sam i poslovno upravljanje u organizaciji Ekonomskog fakulteta Sveu iliata u Zagrebu (engl. Fundamental of Business Administration - FBA). lan sam Hrvatske udruge naftnih in~enjera i geologa (HUNIG) i Society of Petroleum Engineers (SPE), Croatian Section. Polo~ila sam dr~avno-stru ni ispit za obavljanje poslova na rukovodnim radnim mjestima u naftnom rudarstvu u Ministarstvu gospodarstva, rada i poduzetniatva Republike Hrvatske. Trenutno radim na poziciji vodeeg specijalista za ispitivanje stijena i le~ianih fluida u Slu~bi laboratorijskih ispitivanja istra~ivanja i proizvodnje nafte i plina, Sektoru za upravljanje i in~enjering polja, SD Istra~ivanje i proizvodnja nafte i plina, INA, d.d. Poslijediplomski studij upisala sam ak. god. 2004/05. na Rudarsko-geoloako-naftnom fakultetu smjer naftno rudarstvo. PRILOG IV Popis objavljenih radova autora Znanstveni radovi u zbornicima skupova s meunarodnom recenzijom (7) Belamari, I., Jeli Balta, J., Belamari, T. & Greguri, J. (2011): PVT karakterizacija uzorka iz le~iata nafte s plinskom kapom, Prva meunarodna konferencija i izlo~ba o naftno- plinskom gospodarstvu u sredianjoj i isto noj Europi, Sifok, Maarska, (stru ni rad, predavanje) Jeli Balta, J. & Belamari, I. (2011): Optimizacija uvjeta separacije u svrhu maksimiziranja iscrpka le~iata ugljikovodika, Prva meunarodna konferencija i izlo~ba o naftno- plinskom gospodarstvu u sredianjoj i isto noj Europi, Sifok, Maarska, (znanstveni rad, predavanje) Belamari, I., Jeli-Balta, J. & Belamari, T. (2009): Primjena ECM metode na PVT uzorku, Zbornik 4. Meunarodnog znanstveno-stru nog skupa o naftnom gospodarstvu, `ibenik, (znanstveni rad) Belamari, I., Jeli-Balta, J. & Belamari, T. (2009): Provjera konzistentnosti sastava le~ianih i separatorskih fluida Kalinovac-2, Zbornik 4. Meunarodnog znanstveno-stru nog skupa o naftnom gospodarstvu, `ibenik, (stru ni rad) Muvrin, B. & Belamari, I. (2007): Analiza hermeti nosti plinskih procesnih jedinica, 4. meunarodnom znanstveno-stru nom skupu o naftnom rudarstvu; Zadar, (predavanje, stru ni rad) Belamaric, I., Belamaric, T., Perkovic, A. & Sabol, N. (2004): Relational Database as Laboratory Dataset  Base for Qualitative Creation of Reservoir Modelling: WPC 1st Youth Forum, Beijing, China, (poster, stru ni rad) Cibula, I., Jeli-Balta, J. & Gori nik, B. (2003): Experimental and EOS Characterization of Jihar Field Gas Condensate, Zbornik Meunarodnog znanstveno-stru nog skupa o naftnom gospodarstvu, Zadar, (znanstveni rad) Sa~eci u zbornicima skupova (2) ade~, S. & Belamari, I. (2004): GC Method for Separating and Reporting Hydrogen, Helium, Inert Gases and C1-C6 Hydrocarbons in Natural Gas, 18. Hrvatski skup kemi ara i kemijskih in~enjera, Zadar, (poster, sa~etak) ade~, S. & Belamari, I. (2005): Prirodni plin  proairena analiza, 19. Hrvatski skup kemi ara i kemijskih in~enjera, Opatija (poster, sa~etak) Druge vrste radova (3) Jeli-Balta, J., Domitrovi, D., Belamari, I. & Belamari, T. (2004): Correlation Between Injection Gas Properties and Slim Tube Test Recovery of Ivanic Oil, Zbornik radova Ljetna akola naftnog rudarstva, Dubrovnik, (predavanje, stru ni rad) Jeli-Balta, J., Belamari, I. & Belamari, T. (2005): Implementacija suvremene tehnologije u laboratorijskoj praksi INOVA Katalog 30. Hrvatskog salona inovacija, Zagreb, Hrvatski savez inovatora, (stru ni rad, srebrna medalja za inovaciju) Belamari, I., Belamari, T (2004): Baza podataka PVT analiza, Sektor istra~ivanja i razvoja, Zagreb, (predavanje)      PAGE   PAGE XII Uvod  PAGE 160 Teorijsko razmatranje Eksperimentalno istra~ivanje Eksperimentalno istra~ivanje Eksperimentalno istra~ivanje Rezultati istra~ivanja Rezultati istra~ivanja Rezultati istra~ivanja Rezultati istra~ivanja Rezultati istra~ivanja Rezultati istra~ivanja Rezultati istra~ivanja Zaklju ak Literatura  PAGE 185 pr:<>@˻{k^W hi]h +ji h`ih +EHUjS h`ih +EHUVj h`ih +EHUjS h`ih +EHUVh`ih +EHjh`ih +EHUj` h`ih +EHUjS h`ih +EHUVh`ih +EHjh`ih +EHUh`ih +H*h5<2h9hUgh + h`ih +"$&(*  ǺNJ~pg_T~pg_T~phw{h +CJaJh +CJaJh +6CJaJh`ih +6CJH*aJh`ih +6CJaJh`ih +CJaJ!jp h`ih +CJEHUaJ'jS h`ih +CJEHUVaJh`ih +CJEHaJ!jh`ih +CJEHUaJh%MaJmHnHujh`ih)bUaJh`ih +aJ h`ih + 5kdK $$Ifl\ "   t0644 lap(ytdw$$d<<$Ifa$gdV  FHL|~46:bN,.㷮čȅ{tpph h`ih>YBh>YBh>YB6H*h>YBh>YB6h9j h`ih +EHUjS 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ZGGGGG$d$Ifa$gdEzkd;WZ$$IflrS  & &&&& *44 labp2ytEz       ZGGGGG$d$Ifa$gdEzkd ZGGGGG$d$Ifa$gdEzkd=YZ$$IflrS  & &&&& *44 labp2ytEz> @ J V ` n | ZGGGGG$d$Ifa$gdEzkd>ZZ$$IflrS  & &&&& *44 labp2ytEz| ~ n r v    ZTAAAAA$d$Ifa$gdEz$gdkd?[Z$$IflrS  &  & & & &  *44 labp2ytEzx ~                           " $ 0 2 < > B D N P V X ` b n p z | ɸhCJ^JaJnHtH hudh&hudh6CJ]^JaJnHtH hudhCJ^JaJnHtH h6CJH*^JaJnHtH#hxgh6CJ^JaJnHtH&hxgh6CJH*^JaJnHtH8     9&&&$d$Ifa$gdEzkdN\Z$$IflrS  &  & & & &   2*44 labp2ytEz     &kd]Z$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEz      Gkd^Z$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz . < > H T ^ l z Gkd_Z$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzz | ZGGGGG$d$Ifa$gdEzkdaZ$$IflrS  & &&&& *44 labp2ytEz ! ! ! ! ! ! (! *! 4! 6! :! " @" F" H" P" R" ^" `" j" l" hCJ^JaJnHtH hudh hudhCJ^JaJnHtHV ZGGGGG$d$Ifa$gdEzkdbZ$$IflrS  & &&&& *44 labp2ytEz ! ! ! &! 4! ZGGGGG$d$Ifa$gdEzkdcZ$$IflrS  & &&&& *44 labp2ytEz4! 6! @! L! V! d! r! ZGGGGG$d$Ifa$gdEzkddZ$$IflrS  & &&&& *44 labp2ytEzr! t! ~! ! ! ! ! ZGGGGG$d$Ifa$gdEzkdeZ$$IflrS  & &&&& *44 labp2ytEz! ! ! ! ! ! ! ZGGGGG$d$Ifa$gdEzkdfZ$$IflrS  & &&&& *44 labp2ytEz! ! ! " " " ," ZGGGGG$d$Ifa$gdEzkdgZ$$IflrS  & &&&& *44 labp2ytEz," ." 8" D" N" \" j" ZGGGGG$d$Ifa$gdEzkdhZ$$IflrS  & &&&& *44 labp2ytEzj" l" v" " " " " ZGGGGG$d$Ifa$gdEzkdiZ$$IflrS  & &&&& *44 labp2ytEzl" p" r" |" ~" " " " " " " " " " " " " " " " " " " " " " " " " # # # # # # $# &# *# ,# 6# 8# ># @# H# J# V# X# b# d# h# j# t# v# |# ~# # # # # # # # # # # # # # # # # # # # # # # # # $ $ $ $ $ $ "$ $$ hudhhCJ^JaJnHtH hudhCJ^JaJnHtHV" " " " " " " ZGGGGG$d$Ifa$gdEzkd jZ$$IflrS  & &&&& *44 labp2ytEz" " " " # # $# ZGGGGG$d$Ifa$gdEzkd kZ$$IflrS  & &&&& *44 labp2ytEz$# &# 0# <# F# T# b# ZGGGGG$d$Ifa$gdEzkd lZ$$IflrS  & &&&& *44 labp2ytEzb# d# n# z# # # # ZGGGGG$d$Ifa$gdEzkd mZ$$IflrS  & &&&& *44 labp2ytEz# # # # # # # ZGGGGG$d$Ifa$gdEzkd nZ$$IflrS  & &&&& *44 labp2ytEz# # # # $ $ $ ZGGGGG$d$Ifa$gdEzkdoZ$$IflrS  & &&&& *44 labp2ytEz$ $ ($ 4$ >$ L$ Z$ ZGGGGG$d$Ifa$gdEzkdpZ$$IflrS  & &&&& *44 labp2ytEz$$ .$ 0$ 6$ 8$ @$ B$ N$ P$ Z$ \$ `$ b$ l$ n$ t$ v$ ~$ $ $ $ $ $ $ $ $ $ $ $ % % % % % % % % % % % % % % % % % ֳzz&hudh6CJ]^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhhCJ^JaJnHtH hudhCJ^JaJnHtH-Z$ \$ f$ r$ |$ $ $ ZGGGGG$d$Ifa$gdEzkdqZ$$IflrS  & &&&& *44 labp2ytEz$ $ % % % % % % ZTAAAAA$d$Ifa$gdEz$gdkdrZ$$IflrS  &  & & & &  *44 labp2ytEz% % % % % 9&&&$d$Ifa$gdEzkd sZ$$IflrS  &  & & & &   2*44 labp2ytEz% % % % % &kdqtZ$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEz% % % & & & && 2& <& GkduZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz% % % & & & & & & & "& ,& .& 2& 4& 6& >& @& L& N& X& Z& ^& `& j& l& p& r& t& |& ~& & & & & & & & & & & & & & & & & & & & & & & & & & & ' ' ' ' ' ' $' &' *' ,' .' 6' 8' D' F' P' R' V' X' b' d' h' j' hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h%hCJ^JaJnHtHO<& J& X& Z& d& p& z& & & GkdvZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz& & & & & & & ZGGGGG$d$Ifa$gdEzkdwZ$$IflrS  & &&&& *44 labp2ytEz& & & & & ' ' ZGGGGG$d$Ifa$gdEzkdxZ$$IflrS  & &&&& *44 labp2ytEz' ' ' *' 4' B' P' ZGGGGG$d$Ifa$gdEzkdyZ$$IflrS  & &&&& *44 labp2ytEzP' R' \' h' r' ' ' ZGGGGG$d$Ifa$gdEzkdzZ$$IflrS  & &&&& *44 labp2ytEzj' l' t' v' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ( ( ( ( ( ( ( "( $( &( .( 0( <( >( H( J( N( P( Z( \( `( b( d( l( n( z( |( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( hudhCJ^JaJnHtH hudh h%hCJ^JaJnHtHhCJ^JaJnHtHO' ' ' ' ' ' ' ZGGGGG$d$Ifa$gdEzkd{Z$$IflrS  & &&&& *44 labp2ytEz' ' ' ' ' ' ( ZGGGGG$d$Ifa$gdEzkd|Z$$IflrS  & &&&& *44 labp2ytEz ( ( ( "( ,( :( H( ZGGGGG$d$Ifa$gdEzkd}Z$$IflrS  & &&&& *44 labp2ytEzH( J( T( `( j( x( ( ZGGGGG$d$Ifa$gdEzkd~Z$$IflrS  & &&&& *44 labp2ytEz( ( ( ( ( ( ( ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz( ( ( ( ( ( ) ZGGGGG$d$Ifa$gdEzkdۀZ$$IflrS  & &&&& *44 labp2ytEz( ( ( ( ( ) ) ) ) ) ) ) ) ) &) () 4) 6) @) B) F) H) R) T) X) Z) \) d) f) r) t) ~) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) ) * * * * * * * * * ,* .* 8* :* >* @* J* L* P* R* T* \* hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h%hCJ^JaJnHtHO) ) ) ) $) 2) @) ZGGGGG$d$Ifa$gdEzkd܁Z$$IflrS  & &&&& *44 labp2ytEz@) B) L) X) b) p) ~) ZGGGGG$d$Ifa$gdEzkd݂Z$$IflrS  & &&&& *44 labp2ytEz~) ) ) ) ) ) ) ZGGGGG$d$Ifa$gdEzkdރZ$$IflrS  & &&&& *44 labp2ytEz) ) ) ) ) ) ) ZGGGGG$d$Ifa$gdEzkd߄Z$$IflrS  & &&&& *44 labp2ytEz) ) * * * ** 8* ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz8* :* D* P* Z* h* v* ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz\* ^* j* l* v* x* |* ~* * * * * * * * * * * * * * + + + + + + + + + + + + + + + + , , , , , ŽŽŢ}ii&hudh6CJ]^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhCJ^JaJnHtH hudh h%hCJ^JaJnHtHhCJ^JaJnHtH)v* x* * * * * * ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz* * + + + + + + ZTAAAAA$d$Ifa$gdEz$gdkdZ$$IflrS  &  & & & &  *44 labp2ytEz+ + + + + 9&&&$d$Ifa$gdEzkdZ$$IflrS  &  & & & &   2*44 labp2ytEz+ + + + , &kdCZ$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEz, , , *, 8, :, D, P, Z, GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz, , , , , ,, ., 8, :, >, @, J, L, P, R, T, \, ^, j, l, v, x, |, ~, , , , , , , , , , , , , , , , , , , , , , , , , , , - - - - - - - $- &- 0- 2- 6- 8- B- D- H- J- L- T- V- b- d- n- p- t- v- - - - - hudhCJ^JaJnHtH hudhhCJ^JaJnHtH hhCJ^JaJnHtHOZ, h, v, x, , , , , , GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz, , , , , , , ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz, , , - - "- 0- ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz0- 2- <- H- R- `- n- ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzn- p- z- - - - - ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz- - - - - - - - - - - - - - - - - - - - - - - - - . . . . . . . (. *. .. 0. :. <. @. B. D. L. N. Z. \. f. h. l. n. x. z. ~. . . . . . . . . . . . . . . . . . . . . . . . . . . . . hudhCJ^JaJnHtH hudh hhCJ^JaJnHtHhCJ^JaJnHtHO- - - - - - - ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz- - - . . . (. ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz(. *. 4. @. J. X. f. ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzf. h. r. ~. . . . ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz. . . . . . . ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz. . . . / / / ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz. / / / / / "/ &/ (/ 2/ 4/ 8/ :/ 0 J0 L0 V0 X0 \0 ^0 h0 j0 n0 p0 r0 z0 hudhCJ^JaJnHtH hudhhCJ^JaJnHtH hhCJ^JaJnHtHO / "/ ,/ 8/ B/ P/ ^/ ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz^/ `/ j/ v/ / / / ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz/ / / / / / / ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz/ / / / / 0 0 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz0 0 $0 00 :0 H0 V0 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzV0 X0 b0 n0 x0 0 0 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzz0 |0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 $1 &1 1 1 1 1 1 1 1 1 1 1 2 2 2 2 *2 ,2 02 ŽŽŢ}ii&hudh6CJ]^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhCJ^JaJnHtH hudh hhCJ^JaJnHtHhCJ^JaJnHtH)0 0 0 0 0 0 0 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz0 0 1 1 1 1 1 1 ZTAAAAA$d$Ifa$gdEz$gdkdZ$$IflrS  &  & & & &  *44 labp2ytEz1 1 2 2 6##$d$Ifa$gdEzkdĠZ$$IflrS  &  & & & &   2*44 labp2ytEz 2 2 2 2 $d$Ifa$gdEz2 2 $2 02 6##$d$Ifa$gdEzkdZ$$IflrS  & &&&&  2*44 labp2ytEz02 22 42 <2 >2 J2 L2 V2 X2 \2 ^2 h2 j2 n2 p2 r2 z2 |2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 3 3 3 3 3 3 "3 $3 (3 *3 ,3 43 63 B3 D3 N3 P3 T3 V3 `3 b3 f3 h3 j3 r3 t3 3 3 3 3 3 3 3 3 3 3 hudhCJ^JaJnHtH hudhhCJ^JaJnHtH hhCJ^JaJnHtHO02 :2 H2 V2 X2 b2 n2 x2 DkdpZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzx2 2 2 2 2 2 2 2 DkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz2 2 2 2 2 2 3 3 DkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz3 3 3 (3 23 @3 N3 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzN3 P3 Z3 f3 p3 ~3 3 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz3 3 3 3 3 3 3 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 4 4 4 4 4 4 4 "4 $4 ,4 .4 :4 <4 F4 H4 L4 N4 X4 Z4 ^4 `4 b4 j4 l4 x4 z4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 5 5 5 5 5 5 5 5 5 hudhCJ^JaJnHtH hudh hhCJ^JaJnHtHhCJ^JaJnHtHO3 3 3 3 3 3 4 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz4 4 4 4 *4 84 F4 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzF4 H4 R4 ^4 h4 v4 4 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz4 4 4 4 4 4 4 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz4 4 4 4 4 4 5 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz5 5 5 5 "5 05 >5 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz5 $5 &5 25 45 >5 @5 D5 F5 P5 R5 V5 X5 Z5 b5 d5 p5 r5 |5 ~5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 5 6 6 6 6 6 6 6 6 *6 ,6 66 86 <6 >6 H6 J6 N6 P6 R6 Z6 \6 h6 j6 t6 v6 z6 |6 6 6 6 6 6 6 hudhCJ^JaJnHtH hudhhCJ^JaJnHtH hhCJ^JaJnHtHO>5 @5 J5 V5 `5 n5 |5 WDDDDD$d$Ifa$gdEzkdƯZ$$IflrS  & &&&& *44 labp2ytEz|5 ~5 5 5 5 5 5 WDDDDD$d$Ifa$gdEzkd̰Z$$IflrS  & &&&& *44 labp2ytEz5 5 5 5 5 5 5 WDDDDD$d$Ifa$gdEzkdұZ$$IflrS  & &&&& *44 labp2ytEz5 5 6 6 6 (6 66 WDDDDD$d$Ifa$gdEzkdزZ$$IflrS  & &&&& *44 labp2ytEz66 86 B6 N6 X6 f6 t6 WDDDDD$d$Ifa$gdEzkd޳Z$$IflrS  & &&&& *44 labp2ytEzt6 v6 6 6 6 6 6 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz6 6 6 6 6 6 6 6 6 6 6 6 6 6 6 6 6 6 6 7 7 <7 >7 B7 D7 8 8 8 8 8 8 8 .8 08 28 T8 V8 `8 h8 j8 n8 ŽŽŢ}ii&hudh6CJ]^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhCJ^JaJnHtH hudh hhCJ^JaJnHtHhCJ^JaJnHtH(6 6 6 6 6 6 6 WDDDDD$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz6 6 8 8 8 8 8 08 WQ>>>>>$d$Ifa$gdEz$gdkdZ$$IflrS  &  & & & &  *44 labp2ytEz08 28 <8 H8 P8 9&&&$d$Ifa$gdEzkdZ$$IflrS  &  & & & &   2*44 labp2ytEzP8 R8 T8 V8 b8 &kdUZ$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEzb8 n8 x8 8 8 8 8 8 8 GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzn8 p8 r8 z8 |8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 8 9 9 9 9 9 (9 *9 .9 09 29 :9 <9 H9 J9 T9 V9 `9 h9 j9 n9 p9 r9 z9 |9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 9 : : : hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h_| hCJ^JaJnHtHO8 8 8 8 8 8 8 9 9 GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz9 9 "9 .9 89 F9 T9 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzT9 V9 b9 n9 x9 9 9 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz9 9 9 9 9 9 9 ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz9 9 9 9 9 : : ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz: : ": .: 8: F: T: ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz: : : (: *: .: 0: 2: :: <: H: J: T: V: `: h: j: n: p: r: z: |: : : : : : : : : : : : : : : : : : : : : : : : : ; ; ; ; ; (; *; .; 0; 2; :; <; H; J; T; V; `; h; j; n; p; r; z; |; ; ; ; ; ; ; ; ; ; ; h_| hCJ^JaJnHtH hudhCJ^JaJnHtHhCJ^JaJnHtH hudhOT: V: b: n: x: : : ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz: : : : : : : ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz: : : : : ; ; ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz; ; "; .; 8; F; T; ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzT; V; b; n; x; ; ; ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz; ; ; ; ; ; ; ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz; ; ; ; ; ; ; ; ; ; ; ; ; ; ; < < < < < (< *< .< 0< 2< :< << H< J< T< V< `< h< j< n< p< r< z< |< < < < < < < < < < < < < < < < < < < < < < < < < = = = = = (= *= .= 0= 2= := <= H= J= T= V= hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h_| hCJ^JaJnHtHN; ; ; ; ; < < ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz< < "< .< 8< F< T< ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzT< V< b< n< x< < < ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz< < < < < < < ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz< < < < < = = ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz= = "= .= 8= F= T= ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzT= V= f> j> n> x> > > ZTAAAAA$d$Ifa$gdEz$gdkdZ$$IflrS  &  & & & &  *44 labp2ytEzV= f= h= = = = = f> p> v> z> > > > > > > > > > > > > > > > > > > > > ? ? ? ? ? ? ? ? ,? .? 8? ٴzzizizizizzizizizi h_| hCJ^JaJnHtHhCJ^JaJnHtH hudh&hudh6CJ]^JaJnHtH hudhCJ^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh)> > > > > 9&&&$d$Ifa$gdEzkdZ$$IflrS  &  & & & &   2*44 labp2ytEz> > > > > &kd'Z$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEz> > > > > > ? ? ? GkdxZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz? *? 8? :? F? R? \? j? x? GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz8? :? D? L? N? R? T? V? ^? `? l? n? x? z? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? ? @ @ @ @ @ @ @ @ ,@ .@ 8@ :@ D@ L@ N@ R@ T@ V@ ^@ `@ l@ n@ x@ z@ @ @ @ @ @ @ @ @ @ @ @ @ @ @ @ @ @ @ h_| hCJ^JaJnHtH hudhCJ^JaJnHtHhCJ^JaJnHtH hudhOx? z? ? ? ? ? ? ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz? ? ? ? ? ? ? ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz? ? @ @ @ *@ 8@ ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz8@ :@ F@ R@ \@ j@ x@ ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzx@ z@ @ @ @ @ @ ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz@ @ @ @ @ @ @ ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz@ @ @ @ @ @ @ A A A A A A A A ,A .A 8A :A DA LA NA RA TA VA ^A `A lA nA xA zA A A A A A A A A A A A A A A A A A A A A A A A A B B B B B B B B ,B .B 8B :B DB LB NB RB TB VB ^B `B lB nB xB zB B hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h_| hCJ^JaJnHtHO@ @ A A A *A 8A ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz8A :A FA RA \A jA xA ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzxA zA A A A A A ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzA A A A A A A ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzA A B B B *B 8B ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz8B :B FB RB \B jB xB ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzxB zB B B B B B ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzB B B B B B B B B B B B B B B B B B B B B B B B C C C C C C C C ,C .C 8C :C DC LC NC RC TC VC ^C `C lC nC xC zC C C C C C C C C C C C C C C D D D D D ŽŽh%MmHnHujhUh hudh h_| hCJ^JaJnHtHhCJ^JaJnHtH hudhCJ^JaJnHtHBB B B B B B B ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzB B C C C *C 8C ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEz8C :C FC RC \C jC xC ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzxC zC C C C C C ZGGGGG$d$Ifa$gdEzkdZ$$IflrS  & &&&& *44 labp2ytEzC C D D D D D D ZTAAAAA$d$Ifa$gdEz$gdkdZ$$IflrS  &  & & & &  *44 labp2ytEzD D D D D D D D D D E E (E 0E 2E 6E 8E :E BE DE PE RE \E ^E hE pE rE vE xE zE E E E E E E E E E E E E E E E E E E E E ȷ}}}}}}}}}}}} h_| hCJ^JaJnHtHhCJ^JaJnHtH hudh&hudh6CJ]^JaJnHtH hudhCJ^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtH1D D E E E 9&&&$d$Ifa$gdEzkdZ$$IflrS  &  & & & &   2*44 labp2ytEzE E E E *E &kdZ$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEz*E 6E @E NE \E ^E jE vE E GkdJZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzE E E E E E E E E GkdYZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzE E E E F F F ZGGGGG$d$Ifa$gdEzkdZZ$$IflrS  & &&&& *44 labp2ytEzE E E E E F F F F F F (F 0F 2F 6F 8F :F BF DF PF RF \F ^F hF pF rF vF xF zF F F F F F F F F F F F F F F F F F F F F F F F F G G G G G G (G 0G 2G 6G 8G :G BG DG PG RG \G ^G hG pG rG vG xG zG G G G hudh h_| hCJ^JaJnHtH hudhCJ^JaJnHtHhCJ^JaJnHtHOF F *F 6F @F NF \F ZGGGGG$d$Ifa$gdEzkd[Z$$IflrS  & &&&& *44 labp2ytEz\F ^F jF vF F F F ZGGGGG$d$Ifa$gdEzkd\Z$$IflrS  & &&&& *44 labp2ytEzF F F F F F F ZGGGGG$d$Ifa$gdEzkd]Z$$IflrS  & &&&& *44 labp2ytEzF F F F G G G ZGGGGG$d$Ifa$gdEzkd^Z$$IflrS  & &&&& *44 labp2ytEzG G *G 6G @G NG \G ZGGGGG$d$Ifa$gdEzkd_Z$$IflrS  & &&&& *44 labp2ytEz\G ^G jG vG G G G ZGGGGG$d$Ifa$gdEzkd`Z$$IflrS  & &&&& *44 labp2ytEzG G G G G G G G G G G G G G G G G G G G G G H H H H H H (H 0H 2H 6H 8H :H BH DH PH RH \H ^H hH pH rH vH xH zH H H H H H H H H H H H H H H H H H H H H H H H H I I I I I I (I 0I 2I 6I hudhCJ^JaJnHtH hudh h_| hCJ^JaJnHtHhCJ^JaJnHtHOG G G G G G G ZGGGGG$d$Ifa$gdEzkdaZ$$IflrS  & &&&& *44 labp2ytEzG G G G H H H ZGGGGG$d$Ifa$gdEzkdbZ$$IflrS  & &&&& *44 labp2ytEzH H *H 6H @H NH \H ZGGGGG$d$Ifa$gdEzkdcZ$$IflrS  & &&&& *44 labp2ytEz\H ^H jH vH H H H ZGGGGG$d$Ifa$gdEzkddZ$$IflrS  & &&&& *44 labp2ytEzH H H H H H H ZGGGGG$d$Ifa$gdEzkdeZ$$IflrS  & &&&& *44 labp2ytEzH H H H I I I ZGGGGG$d$Ifa$gdEzkdfZ$$IflrS  & &&&& *44 labp2ytEzI I *I 6I @I NI \I ZGGGGG$d$Ifa$gdEzkdgZ$$IflrS  & &&&& *44 labp2ytEz6I 8I :I BI DI PI RI \I ^I hI pI rI vI xI zI I I I I I I I I I I I I I I I I I I I I I I I I J J J J J J .J 0J hJ jJ nJ pJ .K 8K >K BK ŽŽŢ&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h_| hCJ^JaJnHtH6\I ^I jI vI I I I ZGGGGG$d$Ifa$gdEzkdhZ$$IflrS  & &&&& *44 labp2ytEzI I I I I I I ZGGGGG$d$Ifa$gdEzkdiZ$$IflrS  & &&&& *44 labp2ytEzI I I I J J J ZGGGGG$d$Ifa$gdEzkdjZ$$IflrS  & &&&& *44 labp2ytEzJ J .K 2K 6K @K JK \K ZTAAAAA$d$Ifa$gdEz$gdkdkZ$$IflrS  &  & & & &  *44 labp2ytEzBK HK JK LK ZK \K ^K K K K K K K K K K K K K K K K K K K K K K K K K L L L L L L L L &L (L 4L 6L @L BL LL TL VL ZL \L ^L fL hL tL vL L L L L L L L L L L õ޵ޤõ޵ޤõ޵ޤõ޵ޤõ޵ޤ h_| hCJ^JaJnHtHhCJ^JaJnHtH hudh&hudh6CJ]^JaJnHtH hudhCJ^JaJnHtH h6CJH*^JaJnHtH@\K ^K hK tK |K 9&&&$d$Ifa$gdEzkdzZ$$IflrS  &  & & & &   2*44 labp2ytEz|K ~K K K K &kdZ$$IflrS  & &&&&  2*44 labp2ytEz$d$Ifa$gdEzK K K K K K K K K GkdZ$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEzK K L L L L $L 2L @L Gkd+[$$IflrS  & &&&& *44 labp2ytEz$d$Ifa$gdEz@L BL NL ZL dL rL L ZGGGGG$d$Ifa$gdEzkd,[$$IflrS  & &&&& *44 labp2ytEzL L L L L L L ZGGGGG$d$Ifa$gdEzkd-[$$IflrS  & &&&& *44 labp2ytEzL L L L L L L L L L L L L L L M M M M M M M M &M (M 4M 6M @M BM LM TM VM ZM \M ^M fM hM tM vM M M M M M M M M M M M M M M M M M M M M M M M M N N N N N N N N &N (N 4N 6N @N BN LN TN VN hudhCJ^JaJnHtH hudhhCJ^JaJnHtH h_| hCJ^JaJnHtHOL L L L L L M ZGGGGG$d$Ifa$gdEzkd.[$$IflrS  & &&&& *44 labp2ytEzM M M M $M 2M @M ZGGGGG$d$Ifa$gdEzkd/[$$IflrS  & &&&& *44 labp2ytEz@M BM NM ZM dM rM M ZGGGGG$d$Ifa$gdEzkd0[$$IflrS  & &&&& *44 labp2ytEzM M M M M M M ZGGGGG$d$Ifa$gdEzkd1[$$IflrS  & &&&& *44 labp2ytEzM M M M M M N ZGGGGG$d$Ifa$gdEzkd2[$$IflrS  & &&&& *44 labp2ytEzN N N N $N 2N @N ZGGGGG$d$Ifa$gdEzkd3[$$IflrS  & &&&& *44 labp2ytEz@N BN NN ZN dN rN N ZGGGGG$d$Ifa$gdEzkd4 [$$IflrS  & &&&& *44 labp2ytEzVN ZN \N ^N fN hN tN vN N N N N N N N N N N N N N N N N N N N N N N N N O O O O O O O O &O (O 4O 6O @O BO LO TO VO ZO \O ^O fO hO tO vO O O O O O O O O O O O O O O O O O O O O O O O O hudhhCJ^JaJnHtH h_| hCJ^JaJnHtH hudhCJ^JaJnHtHON N N N N N N ZGGGGG$d$Ifa$gdEzkd5 [$$IflrS  & &&&& *44 labp2ytEzN N N N N N O ZGGGGG$d$Ifa$gdEzkd6 [$$IflrS  & &&&& *44 labp2ytEzO O O O $O 2O @O ZGGGGG$d$Ifa$gdEzkd7 [$$IflrS  & &&&& *44 labp2ytEz@O BO NO ZO dO rO O ZGGGGG$d$Ifa$gdEzkd8 [$$IflrS  & &&&& *44 labp2ytEzO O O O O O O ZGGGGG$d$Ifa$gdEzkd9[$$IflrS  & &&&& *44 labp2ytEzO O O O O O P ZGGGGG$d$Ifa$gdEzkd:[$$IflrS  & &&&& *44 labp2ytEzO P P P P P P P P &P (P 4P 6P @P BP LP TP VP ZP \P ^P fP hP tP vP P P P P P P P P Q Q Q Q Q Q Q Q Q ŽŽŢ}ii&hudh6CJ]^JaJnHtH h6CJH*^JaJnHtH&hxgh6CJH*^JaJnHtH#hxgh6CJ^JaJnHtHh%MmHnHujhUh hudhCJ^JaJnHtHhCJ^JaJnHtH hudh h_| hCJ^JaJnHtH)P P P P $P 2P @P ZGGGGG$d$Ifa$gdEzkd;[$$IflrS  & &&&& *44 labp2ytEz@P BP NP ZP dP rP P ZGGGGG$d$Ifa$gdEzkd<[$$IflrS  & &&&& *44 labp2ytEzP P Q Q Q Q Q Q ZTAAAAA$d$Ifa$gdEz$gdkd=[$$IflrS  &  & & & &  *44 labp2ytEzQ Q Q Q Q 9&&&$d$Ifa$gdEzkdL[$$IflrS  &  & & & &   2*44 labp2ytEzQ Q Q Q Q Q Q R R R R R R R &R (R 2R :R Y LY ZGGGGG$d$Ifa$gdEzkd.[$$IflrS  & &&&& *44 labp2ytEzLY NY ZY fY pY ~Y Y ZGGGGG$d$Ifa$gdEzkd/[$$IflrS  & &&&& *44 labp2ytEzY Y Y Y Y Y Y ZGGGGG$d$Ifa$gdEzkd0[$$IflrS  & &&&& *44 labp2ytEzY Y Y Y Y Y Z ZGGGGG$d$Ifa$gdEzkd1[$$IflrS  & &&&& *44 labp2ytEz Z Z Z &Z 0Z >Z LZ ZGGGGG$d$Ifa$gdEzkd2[$$IflrS  & &&&& *44 labp2ytEzLZ NZ ZZ fZ pZ ~Z Z ZGGGGG$d$Ifa$gdEzkd3[$$IflrS  & &&&& *44 labp2ytEzNZ XZ `Z bZ fZ hZ jZ rZ tZ Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z Z [ [ [ [ [ [ "[ &[ ([ *[ 2[ 4[ @[ B[ L[ N[ X[ `[ b[ f[ h[ j[ r[ t[ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ [ hudh h_| hCJ^JaJnHtH hudhCJ^JaJnHtHhCJ^JaJnHtHOZ Z Z Z Z Z Z ZGGGGG$d$Ifa$gdEzkd4[$$IflrS  & &&&& *44 labp2ytEzZ Z Z Z Z Z [ ZGGGGG$d$Ifa$gdEzkd5[$$IflrS  & &&&& *44 labp2ytEz [ [ [ &[ 0[ >[ L[ ZGGGGG$d$Ifa$gdEzkd6[$$IflrS  & &&&& *44 labp2ytEzL[ N[ Z[ f[ p[ ~[ [ ZGGGGG$d$Ifa$gdEzkd7[$$IflrS  & &&&& *44 labp2ytEz[ [ [ [ [ [ [ ZGGGGG$d$Ifa$gdEzkd8[$$IflrS  & &&&& *44 labp2ytEz[ [ [ [ [ [ \ ZGGGGG$d$Ifa$gdEzkd9[$$IflrS  & &&&& *44 labp2ytEz[ [ \ \ \ \ \ \ "\ &\ (\ *\ 2\ 4\ @\ B\ L\ N\ X\ `\ b\ f\ h\ j\ r\ t\ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ \ ] ] ] ] ] ] "] &] (] *] 2] 4] @] B] L] N] P] R] T] V] Ŀķh[heJ5 h[5 heJ5 hudhCJ^JaJnHtH hudh h_| hCJ^JaJnHtHhCJ^JaJnHtHE \ \ \ &\ 0\ >\ L\ ZGGGGG$d$Ifa$gdEzkd:[$$IflrS  & &&&& *44 labp2ytEzL\ N\ Z\ f\ p\ ~\ \ ZGGGGG$d$Ifa$gdEzkd;[$$IflrS  & &&&& *44 labp2ytEz\ \ \ \ \ \ \ ZGGGGG$d$Ifa$gdEzkd<[$$IflrS  & &&&& *44 labp2ytEz\ \ \ \ \ \ ] ZGGGGG$d$Ifa$gdEzkd=[$$IflrS  & 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