ࡱ> JuwjklmnopqrstUv ~ N P R TXZikmoqsRTVkTVXik !!p"#\##_$`x{bjbjss  W'h 8VL)}#(f HBDxxxxxxx$~h7:*xxHHxx*x f |MMMxf7 z f xMxxMMdx hff v PI_%X!> EMBED Equation.DSMT4  tj. sistem odgovara sa karakteristi nim relaksacijskim vremenom, dakle na puno ni~im frekvencijama ( EMBED Equation.DSMT4 ) od vlastite frekvencije , tj.  EMBED Equation.DSMT4 << EMBED Equation.DSMT4 . Dakle, jednad~ba (3.25) u limesu  EMBED Equation.DSMT4  postaje Debyeva funkcija:  EMBED Equation.DSMT4  (3.27) U realnim sistemima koje prou avamo, pojavljuje se distribucija relaksacijskih vremena oko srednjeg vremena relaksacije; . Takve sisteme bolje opisuje poopena Debyeva funkcija: Havriliak- Negami funkcija  EMBED Equation.3 :   MACROBUTTON MTEditEquationSection2 Equation Section (Next) SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \h \* MERGEFORMAT (3.28) gdje parametar  EMBED Equation.DSMT4  opisuje airinu distribucije (ato je  EMBED Equation.DSMT4  manji, to je aira distribucija).  opisuje jakost dielektri ne relaksacije istra~ivanog sistema. Pojedina kompleksna HN funkcija se eksplicitno rastavlja na imaginarnu i realnu komponentu:  EMBED Equation.DSMT4   MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 18 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 18 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 18 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 18 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT (3.29)  EMBED Equation.DSMT4  (3.30) Ako imamo viae od jednog relaksacijskog procesa, Havriliak- Negami funkcije se upotrebljavaju aditivno; npr. u slu aju dva relaksacijska procesa:   MACROBUTTON MTEditEquationSection2 Equation Section (Next) SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \h \* MERGEFORMAT (3.31)  EMBED Equation.DSMT4  Prilagodba rezultata- tehni ki detalji Oduzimanje pozadine vodenog elektrolita uklanja vodljivost slobodnih nosioca Gbg i njihov doprinos kapacitetu Cbg. Meutim, kako se referentna otopina ne mo~e izabrati tako da se admitancija savraeno poklapa, uvijek e postajati mali, neuklonjeni dio Gbg i Cbg. Kako je razlog isto tehni ke prirode, te varijable ozna avamo kao  i .  se o itava ru no, na najni~im frekvencijama na kojima podaci za G ne pokazuju zna ajnu ovisnost o frekvenciji. Najbolja provjera izbora  je vidjeti da li niz podataka za  pokazuje simetri no-zvonolik oblik, u kojem slu aju je izbor  prihvatljiv (poglavlje 4.3). Neuklonjeni kapacitet javlja se u dielektri noj funkciji kao  EMBED Equation.DSMT4  i uvodimo ga u prilagodbu kao slobodni parametar. Podaci dobiveni pomou izraza (3.14) i (3.15) korigiraju se na sljedei na in:  EMBED Equation.DSMT4  (3.32)  EMBED Equation.DSMT4  (3.33) Na realnu i imaginarnu komponentu Havriliak- Negami funkcije prilagoavaju se korigirani podaci iz izraza (3.32) i (3.33). Kada imamo dva relaksacijska procesa, izraze (3.29) i (3.30) za prilagodbu proairimo pomou izraza  GOTOBUTTON ZEqnNum634591 \* MERGEFORMAT (3.31):  EMBED Equation.DSMT4  (3.34)  EMBED Equation.DSMT4  (3.35) Numeri ki, ova prilagodba se izvodi u kompleksnoj ravnini- ne prilagoava se zasebno na podatke za realni i imaginarni dio tj. i realni i imaginarni dio pojedinog dielektri nog moda opisan je sa tri parametra:  EMBED Equation.DSMT4 ,  EMBED Equation.DSMT4 ,  EMBED Equation.DSMT4 . 3.5 OPIS ELEKTRI NE SHEME MJERENJA Frekventna ovisnost realnog dijela admitancije i kapaciteta mjeri se preciznim analizatorom impedancije Agilent 4294A. Mjerno podru je frekvencija je 40 Hz- 110 MHz. Mjeri se, uz postavku BW=1, 27 frekvencija po dekadi, usrednjava 10 puta na jednoj to ki i zatim se cijeli spektar mjeri 3 puta i usrednjava (radi uklanjanja utjecaja varijacija temperature uzorka). Odgovarajuom shemom (slika 3.2), dvije Pt- elektrode spojene su na osam elektri nih konekcijskih mjesta ( etiri centralna voda + etiri oklopa) na Agilent ureaju. Ova shema preporu a se od proizvoa a instrumenta radi uklanjanja parazitnih impedancija (put signala i naponski kablovi su meusobno neovisni)  EMBED Equation.3 . Sama komora je spojena direktno na Agilent odgovarajuim BNC konektorima ugraenim na tijelo komore (oznake BNC konektora su: LCUR- strujni minus, LPOT- naponski minus, HPOT- naponski plus, HCUR- strujni plus). Iz konektora kroz komoru prolaze etiri tanka koaksijalna kabla (slika 3.2). Njihovi centralni vodi i spajaju se dva i dva ( LCUR sa LPOT, HCUR sa HPOT), kako bi ih se dalje spojilo na dvije Pt- elektrode. Kako povratna struja te e kroz vanjski vodi  koaksijalnog kabla, magnetsko polje generirano od unutraanjeg vodi a se poniatava onim od vanjskog vodi a (oklop). Od mjesta spojeva do Pt- elektroda vodi neoklopljena, lakirana bakrena ~ica. Kako bi mjerenje bilo ato preciznije, a parazitski kapaciteti ato manji, put signala od Agilenta do uzorka mora biti ato krai. Dakle, du~ina neoklopljenih, lakiranih bakrenih ~ica treba biti ato manja. Klju ni zahtjev u shemi je spojiti oklope koaksijalnih kablova ato je mogue bli~e Pt- elektrodama ato je postignuto uvoenjem koaksijalnih kablova bez vanjske izolacije oklopa u tijelo komore koje tada slu~i kao oklop. Centralni vodovi kablova su provu eni kroz tijelo komore i spojeni u parovima na Pt- elektrode. Tako plo e elektroda postaju jedini izvor impedancije, uz uzorak.    SHAPE \* MERGEFORMAT  Slika 3.2: Shematski prikaz spajanja Pt  elektroda i etiri konektora na prednjoj plo i analizatora impedancije Agilent 4294A pomou koaksijalnih kablova i BNC  konektora. 1. Koaksijalni kablovi, 2. BNC konektori, 3. Centralni vodovi: izvan oklopa, ali unutar kuiata komore. Prikazana shema omoguava uklanjanje svih parazitskih impedancija uzrokovanih kablovima i konektorima. Slika 3.3 prikazuje pojednostavljeni elektri ni sklop Agilenta 4294A i uzorka. Ja ina signala kroz uzorak ovisi o naponskom signalu Agilenta 4294A,  EMBED Equation.DSMT4 , unutarnjem otporu Agilenta 4294A,  EMBED Equation.DSMT4 , i impedanciji uzorka,  EMBED Equation.DSMT4 :  EMBED Equation.DSMT4   MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT (3.36)  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 24 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 24 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT   EMBED Equation.DSMT4   MACROBUTTON MTEditEquationSection2 Equation Chapter 3 Section 25 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 25 \h \* MERGEFORMAT  SEQ MTChap \r 3 \h \* MERGEFORMAT (3.37)  EMBED Equation.DSMT4  gdje je  EMBED Equation.DSMT4  naponski signal na uzorku,  EMBED Equation.DSMT4  struja koja te e kroz uzorak. Ureaj automatski podeaava  EMBED Equation.DSMT4 . Mi smo odabrali  EMBED Equation.DSMT4 , nakon ato smo ustanovili da u podru ju 20- 500mV nema nelinearnosti tj. ovisnosti mjerene impedancije o naponu. Najmanji napon nije odabran zbog prevelikog auma.  EMBED Visio.Drawing.11  Slika 3.3: Pojednostavljeni model principa mjerenja napona na uzorku i struje koja te e kroz uzorak. 3.6 OPIS TEMPERATURNE KONTROLE Sustav za stabilizaciju i kontrolu temperature uzorka radi na osnovi Peltierovih elemenata (podru je:  EMBED Equation.DSMT4 , stabilnost:  EMBED Equation.DSMT4 ), silicijeve diode Si-1000 i platinskog Pt-100 termometra (oznake 1000 i 100 predstavljaju otpore tih termometara na sobnoj temperaturi). Peltierovi elementi i silicijeva dioda Si-1000 nalaze se s vanjske strane kuiata u sklopu termoregulacijskih blokova. Peltierovi elementi su poluvodi ki elementi koji rade kao toplinske pumpe i slu~e za grijanje/hlaenje komore. Silicijeva dioda Si-1000 slu~i pri stabilizaciji temperature (slika 3.4). Temperatura na kojoj se izvodi mjerenje posti~e se izborom kontrolnog napona koji se ru no podeaava potenciometrom na prednjoj plo i ureaja MVTC-402 (u rasponu od -2V do 2V sa minimalnim korakom od 1 mV) te se, u ureaju, taj napon usporeuje sa padom napona na Si- diodi (Si- dioda je otporni termometar otpora 1000 &! na sobnoj temperaturi, svaka promjena temperature komore uzrokuje promjenu otpora, odnosno pada napona na Si- diodi). U ovisnosti o predznaku razlike tih napona, MVTC-402 aalje struju grijanja/hlaenja na Peltierove elemente. Stabilizirana temperatura komore mjeri se Pt- 100 termometrom (to je platinski otpornik otpora 100 &! na sobnoj temperaturi) koji se nalazi unutar kuiata, blizu Pt- elektroda, a o itava se na posebnom ureaju (Ahlborn MA 4490-2).  Slika 3.4: Shema temperaturne kontrole Kako bi Peltierovi elementi efikasno pumpali toplinu u komoru ili iz komore, potreban je vanjski spremnik topline velikog kapaciteta, tj. temperature nepromjenjive pumpanjem (slika 3.5). Ulogu spremnika imaju aluminijski blokovi koji su na Peltierove elemente pri vraeni termi ki vodljivom pastom. Kako bi se odr~ala stalna temperatura aluminijskih blokova, kroz njih protje e voda. U slu aju kada je potrebno komoru grijati na temperaturu viau od sobne, Peltier element grije komoru, a hladi aluminijski blok (pumpa toplinu prema komori). Kada komoru hladimo, Peltier element grije aluminijski blok (pumpa toplinu iz komore).    SHAPE \* MERGEFORMAT  Slika 3.5: Shematski prikaz komore: 1. mesingano ku iate, 2. Al plo ice, 3. platinske elektrode, 4. uzorak, 5. Al blokovi, 6. Peltierovi elementi, 7. cijevi za protok vode, 8. elasti na folija, 9. Si  dioda.10. . Pt  100 termometar.  MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 1 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 1 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT 4. EKSPERIMENTALNO ISTRA}IVANJE MODELNOG KOLOIDA 4.1 UZORCI- POLISTIRENSKI LATEKS Koloidne disperzije su otopine u kojima su molekule otopljene tvari, disperzirane u otapalu, mnogo vee od molekula otapala. Koloidne estice se grubo definiraju kao one estice ija je linearna dimenzija u rasponu 10- 1000 nm. U standardnom ud~beniku za koloide Hunter  EMBED Equation.DSMT4  polazi se od Freundlichove klasifikacije koloida. Freundlich (1926.) je predlo~io da se koloidne disperzije u tekuinama podijele u dva razreda: liofilne (obavijaju se molekulama otapala) i liofobne (ne obavijaju se molekulama otapala); ovisno o lakoi sa kojom se sistem mo~e redisperzirati ako se prethodno osuai. Daljnje istra~ivanje otkrilo je itav niz prijelaznih tipova, ali Freundlichova klasifikacija je joa korisna za razlu ivanje ekstrema. Kruyt (1952.) je upotrijebio istu klasifikaciju i povezao s njom reverzibilne i ireverzibilne sisteme. Ta terminologija jasnije izra~ava pravu prirodu razlike jer ultimativni test da li je sistem liofilan je odreivanje da li se proces disperzije odvija spontano kada se otapalo doda koloidu. U podru ju izmeu dva ekstrema le~e sistemi koji mogu pokazati i jedno i drugo ponaaanje. Kada je disperzno sredstvo voda, koriste se nazivi hidrofilni i hidrofobni koloidi. Stabilnost koloidnih estica podrazumijeva sprije avanje agregacije. To se posti~e na dva na ina: nabojnom stabilizacijom i steri kom stabilizacijom. Steri ka stabilizacija se zasniva na prekrivanju povraine liofobne koloidne estice sa liofilnim materijalom polimerne prirode. Kada se dvije takve estice pribli~e, interakcija izmeu adsorbiranih lanaca polimera uzrokuje odbijanje estica koje mo~e biti dovoljno da sprije i agregaciju i tako uzrokuje stabilnost. Nabojnoj stabilizaciji osnova je elektrostatsko odbijanje istoimenih naboja. Mnoge koloidne estice imaju naboj koji dolazi npr. od disocijacije grupa kiselina ili baza na povraini estice. Disperzija tih estica je stabilna i ne dolazi do agregacije jer se estice elektrostatski odbijaju. Povrainski naboj estice djelomi no je zasjenjen protuionima (ioni elektrolita iji je naboj suprotan naboju estice). Polistirenski lateks na kojem je izvraeno naae mjerenje poznati je modelni koloidni sistem. estice (kuglice) polistirena disperzirane u vodi nazivaju lateksom tj. polistirenskim lateksom koji je zaista mlije nog izgleda. Lateks je organski polimer (mlije ni sok nekih tropskih biljaka) koji sadr~i kuglice ije su dimenzije usporedive sa valnom duljinom svjetlosti pa rasprauju svjetlost na sve strane te je zato lateks mlije nog izgleda. Strukturno, polistiren je dugi ugljikovodikov lanac s fenilnom skupinom vezanom na svaki drugi ugljikov atom. Polistirenske mikrosfere su zbog mnogo razloga idealne koloidne estice. Za geometrijski oblik sfere mnoge kemijske i fizikalne karakteristike mogu se lako izra unati jer su mikrosfere monodisperzne ato zna i da su sve sfere pribli~no jednake veli ine. Isto tako, masa i opti ka svojstva su uniformna od sfere do sfere. 4.1.1 PROIZVOA KA SPECIFIKACIJA LATEKSA Naae istra~ivanje izvraili smo na lateksu, airokog raspona promjera kuglica: 56, 210, 400, 1000 nm, nabavljenom od Interfacial Dynamics Corporation, SAD. Lateks je specifi an po tretmanu povraine. To je karboksil (COOH)- modificirani lateks sa -COO- grupama na povraini kuglica. Suhe polistirenske kuglice (suhi lateks) su nabojno neutralne. Naboj kuglica lateksa uzrokovan je disocijacijom karboksilnih grupa na povraini ime se otpuataju protuioni koji ine ionsku protuatmosferu lateksa. Takav lateks omoguava kontrolu protuionske atmosfere te karakterizaciju povraine sfera. Stabilnost sfera je omoguena s velikim nabojem povraine (povrainski naboj) kojeg uzrokuje disocijacija karboksilnih grupa na povraini sfera. Povraina ima veliku gustou karboksila sadr~anog u polimeru oko amorfne polistirenske jezgre. Sloj je hidrofilan i ima trodimenzionalni karakter. Povrainski presjek neioniziranih COOH grupa je 19 2 . U ovom radu prou avamo nabijenu kuglicu lateksa koju okru~uju protuioni (slika 4.1) i njihovo gibanje u elektri nom polju.  SHAPE \* MERGEFORMAT  Slika 4.1: Prikaz negativno nabijene kuglice lateksa okru~ene protuionima pozitivnog naboja. Oznaka  ozna ava -COO- skupine na povraini kuglice dok oznaka + ozna ava protuione. Proizvoa  je odredio promjer i standardnu devijaciju promjera skenirajuim elektronskim mikroskopom (slika 4.2). Sadr~aj karboksila odreen je titracijom. Dobivena vrijednost izra~ena je u mikroekvivalentima Eq po gramu suhog lateksa gdje su mikroekvivalenti jednaki umnoaku naboja i koncentracije estice izra~ene u mol/L tj. u M. Volumni udio vrstog polimera odreen je suhim vaganjem.  SHAPE \* MERGEFORMAT  Slika 4.2: Prikaz kuglica lateksa dobiven elektronskim mikroskopom. Proizvoa ka specifikacija lateksa navedena je u tablici 4.1. 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TTT t0$644 laTccccccccccccccd d dddddd dNdPdRdTdXd\d^ddddd,e.e0e2e8e:ehejelenereteve|e~eeeji h$eh'IEHU hZh'I h'IH*jh$eh'IEHUjh$eh'IEHU!j8H h'ICJPJUVaJj1h$eh'IEHU!j%H h'ICJPJUVaJjh'IUh'Ih$eh'IH* h'IH*2d^d`dddd1kd; $$IfTlr ,<$D TTT t0$644 laT$$Ifa$gd'Ildddd2eve1kd $$IfTlr ,<$D TTT t0$644 laT$$Ifa$gd'Ileeeeeeeeeeeeeeef000406080:0>0@0B0000000000000000,1p1t1v1x1x2z22223.3ȻȬ槙摌h&g h'I6hr/h'I6 h$h'I hth'I h'IH*jsh$eh'IEHUUjh$eh'IEHU!j8H h'ICJPJUVaJh$eh'IH* h'IH*h'Ijh'IUj h$eh'IEHU4veeeB0D001kd!$$IfTlr ,<$D TTT t0$644 laT$$Ifa$gd'Il,8 EMBED Equation.DSMT4 106povraina po 1 karboksilnoj skupini (PA)39 2/COOH61 2/COOH26 2/COOH46 2/COOHpKa5555 Tablica 4.1: Proizvoa ka specifikacija lateksa. Disocijacijom karboksilnih grupa, koloidne estice se nabiju negativno te ih okru~i sloj protuiona. Protuione ini kombinacija H+ i Na+ iona. Karboksilne grupe disociraju kao slaba kiselina:  EMBED Equation.DSMT4   MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 1 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 1 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT (4.1) te se konstanta disocijacije, Ka definira kao:  MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 2 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 2 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT  EMBED Equation.DSMT4  (4.2) MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 2 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 2 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 2 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 2 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT  MACROBUTTON MTEditEquationSection2 Equation Chapter 4 Section 2 SEQ MTEqn \r \h \* MERGEFORMAT  SEQ MTSec \r 2 \h \* MERGEFORMAT  SEQ MTChap \r 4 \h \* MERGEFORMAT  gdje su koncentracije izra~ene u mol/L tj. u M, a ozna avaju se kvadratnim zagradama. Proizvoa  specificira pKa kao 5 (pKa kiseline se izra una pomou:  EMBED Equation.DSMT4 ). 4.2 SASTAV PROTUIONSKE ATMOSFERE LATEKSA 4.2.1 NEDIJALIZIRANI LATEKS Nedijalizirani lateks analiziran je u seminarskom radu Brune Frke- Peteaia (tablica 4.2)  EMBED Equation.DSMT4 . Na osnovu vodljivosti izmjerene u komori,  EMBED Equation.DSMT4 i kemijske elementarne analize, izra unata je koncentracija H+ i Na+ iona (po proizvoa koj specifikaciji ti ioni ine protuionsku atmosferu lateksa). EMBED Equation.DSMT4 . 2R (nm) EMBED Equation.DSMT4  EMBED Equation.DSMT4 ( EMBED Equation.DSMT4 ) EMBED Equation.DSMT4 ( EMBED Equation.DSMT4 ) EMBED Equation.DSMT4 56167,20,03-0,241-34,5221041,50,02-0,030,5-0,74,57400104,00,01-0,071-24,90100040,10,010,74,98 Tablica 4.2: Vodljivosti  EMBED Equation.DSMT4  izmjerene u komori te na temelju njih izra unate koncentracije H+ i Na+ iona te pH za nedijalizirane latekse  EMBED Equation.DSMT4 . Naknadno napravljena elementarna analiza nedijaliziranog lateksa promjera estica 56 nm provedena je kromatografijom ionske mobilnosti. Analizirano je 500 L lateksa kojemu je dodano 10 mL mili Q vode (voda deionizirana filtracijom kroz smolu, te sterilizirana UV zra enjem). Ostale latekse tom metodom nije bilo mogue analizirati zbog veli ine koloidnih estica. Elementarnom analizom nedijaliziranog lateksa 56 nm ustanovljena je stvarna koncentracija iona Na+ koja je sukladna vrijednostima dobivenim u prethodnom radu B. Frke- Peteaia  EMBED Equation.DSMT4 . Dobiveni rezultati prikazani su u tablici 4.3: IonmMCa2+0,03K+0,02Mg2+0,03Na+ 0,9 Tablica 4.3: Rezultati elementarne analize nedijaliziranog lateksa promjera estica 56 nm. 4.2.2 DIJALIZIRANI LATEKS Kako bi olakaali kasniju interpretaciju rezultata pokuaali smo dijalizom ukloniti Na+ ione i zamijeniti ih sa H+ ionima, dakle dobiti isti H lateks. Dijaliza je odvajanje otopljenih tvari iz koloidne otopine pomou membrana vrlo finih pora. Kroz takve membrane prolaze ioni, a zaostaju estice koloidnih dimenzija. Dijalizom odstranjujemo ione Na+ koje bi trebali zamijeniti H+ ioni nastali protolizom vode:  EMBED Equation.DSMT4  koja se spontano odvija kako bi se o uvala neutralnost lateksa (slika 4.3).  SHAPE \* MERGEFORMAT  Slika 4.3: Pojednostavljen prikaz dijalize lateksa. Latekse smo dijalizirali u miliQ vodi. Kao membrane za dijalizu koristili smo celulozna crijeva prethodno prokuhana u miliQ vodi. 500 L lateksa 56 nm, 210 nm, 400 nm, 1000 nm dijalizirano je u 2 L miliQ vode 48 sati. Tablica 4.4 prikazuje dobivene rezultate za dijalizirane latekse. 2R (nm) EMBED Equation.DSMT4 (mM)(pH)pKa=5 EMBED Equation.DSMT4  EMBED Equation.DSMT4  EMBED Equation.DSMT4 ( EMBED Equation.DSMT4 ) EMBED Equation.DSMT4 pKa5619,13,36800,273,575,422103,133,7737,70,133,95,284003,793,7277,70,263,594,7210000,864,0658,80,23,714,24 Tablica 4.4: Rezultati dobiveni nakon dijalize lateksa. U nastavku teksta opisano je zna enje pojedine veli ine. Vodljivost  EMBED Equation.DSMT4 je vodljivost izmjerena u komori. Koncentracija  EMBED Equation.DSMT4 je izra unata na temelju vodljivosti izmjerene u komori, uva~avajui da je koncentracija  EMBED Equation.DSMT4  jednaka koncentraciji  EMBED Equation.DSMT4  iona koja bi uzrokovala izmjerenu vodljivost uzorka uzimajui u obzir da 1 mM (M=mol/L) H+ prenosi vodljivost 300 S/cm (koristimo izraz:  EMBED Equation.DSMT4 gdje je c koncentracija u EMBED Equation.DSMT4 , a  EMBED Equation.DSMT4 je molarna vodljivost,  EMBED Equation.DSMT4   EMBED Equation.DSMT4 ),  EMBED Equation.DSMT4  je izra unat pomou izraza:  EMBED Equation.DSMT4 .  EMBED Equation.DSMT4  je ukupna koncentracija karboksilnih estica izra unata na temelju podataka iz tablice 4.1:  EMBED Equation.DSMT4 . Karboksile razdvojimo na disocirane i nedisocirane:  EMBED Equation.DSMT4  (4.3) Poato su lateksi pripremljeni u istoj vodi, svi H+ bi trebali dolaziti od disocijacije karboksilne kiseline, tj. tada je  EMBED Equation.DSMT4 . Konstanta disocijacije, izraz (4.2), se koristei izraz (4.3) mo~e zapisati :  EMBED Equation.DSMT4  (4.4) Dobiveni pKa bliski su specificiranom pKa= 5. Obrnuto, koristei pKa= 5 (navedeno od proizvoa a, tablica 4.1) mo~emo iz izraza (4.4) dobiti koncentraciju  EMBED Equation.DSMT4 . Odgovarajui pH dani su u drugoj koloni tablice 4.4. Dobiveni rezultati su konzistentni u smislu da su vrijednosti pH dobivene iz vodljivosti kao i one dobivene iz pKa pribli~no jednake. IonmMCa2+1,04K+0,02Mg2+0,15Na+0,15 Tablica 4.5: Rezultati elementarne analize dijaliziranog lateksa 56 nm Tablica 4.5 prikazuje rezultate elementarne analize za dijalizirani lateks. Dobiveni rezultati, zbog velike koncentracije Ca2+ iona, opovrgavaju pretpostavku na temelju koje je, preko vodljivosti (tablica 4.4), raena analiza H+ koncentracija. Dakle, doalo je do ionske izmjene tj. ioni Na+ zamjenjeni su ionima Ca2+ iz vode u kojoj je vraena dijaliza tj. dobili smo Ca lateks umjesto ~eljenog H lateksa. Naknadno smo utvrdili da se kod pripreme posua i mambrana za dijalizu treba koristiti i EDTA kako bi se izbjegla ionska izmjena. EDTA (etilendiamintetraoctena kiselina) koji tvori kompleksan spoj sa ionima Ca2+ i na taj na in uklanja ione Ca2+ iz vode. 4.3 REZULTATI DOBIVENI NFDS Sagledamo li rezultate elementarne analize zaklju it emo da se nedijalizirani i dijalizirani lateks mogu promatrati kao Na i Ca lateksi sa manjim, ako ne i zanemarivim udjelom H+ iona. Prikaz rezultata niskofrekventne dielektri ne spektroskopije (NFDS) bit e usmjeren ka ustanovljavanju postoji li promjena u dielektri nim svojstvima lateksa izazvana izmjenom iona. Prikazat emo proceduru obrade podataka NFDS na jednom reprezentativnom Ca lateksu promjera estica 210 nm te kona ne rezultate za Na i Ca latekse promjera estica 56 nm, 210 nm, 400 nm, 1000 nm. Slika 4.1 prikazuje rezultate mjerenja vodljivosti G i kapaciteta C (vidi podpoglavlje 3.3). Na niskim frekvencijama vidljiv je efekt polarizacije elektroda (detaljno analiziran u podpoglavlju 2.2) dok se na visokim frekvencijama uo avaju rezonantne pojave  EMBED Equation.DSMT4 . Mjerenjem vodljivosti i kapaciteta pozadine (referentna otopina NaCl) nastojimo ukloniti spomenute efekte.  Slika 4.1: Frekventne ovisnosti realnog dijela vodljivosti Gexp i kapaciteta Cexp Ca lateksa 210 nm (puna linija) te realnog dijela vodljivosti GNaCl i kapaciteta CNaCl NaCl otopine (crtkana linija). Eksperimentalni podaci prikazani su linijama zbog velike gustoe podataka. Frekventne ovisnosti vodljivosti i kapaciteta prikazane su u logaritamskoj skali kako bi se prikazao cijeli spektar. Kao pozadina je uzet jednostavni elektrolit - NaCl otopina odgovarajue koncentracije, pa tako i vodljivosti i kapaciteta koji odgovaraju ionskoj vodljivosti lateksa Glateks(100 kHz) te kapacitetu lateksa Clateks(100 Hz). Na slici c) dan je uvean prikaz na linearnoj vertikalnoj skali kako bi se prikazalo podru je najveeg odstupanja kapaciteta uzorka od kapaciteta pozadine. Na slici 4.2 prikazan je rezultat uklanjanja doprinosa pozadine uz pomo izraza 3.7 i 3.9. Odgovarajua otopina NaCl izabere se iz tablice. Tablica se formira tako da se izmjere G i C niza otopina NaCl koncentracija 0,003, 0,01, 0,03, 0,1, 0,3, 1, 3, 10 mM na odreenoj temperaturi. Za meukoncentracije (30 izmeu dviju izmjerenih) se izvodi linearna interpolacija. Time se dobiva tablica u kojoj su zabilje~eni spektri vodljivosti i kapaciteta NaCl (GNaCl i CNaCl). Iz dobivene tablice biramo otopinu NaCl ija je vodljivost na 100 kHz i kapacitet na 100 Hz ato bli~e vodljivosti i kapacitetu uzorka. Vodljivost se o itava na 100 kHz jer je tu doprinos slobodnih nosilaca naboja najmanje pod utjecajem polarizacije elektroda i parazitskih impedancija, a upravo vodljivost slobodnih nosilaca ~elimo ukloniti oduzimanjem GNaCl. Kapacitet se usporeuje na 100 Hz tj. podeaavamo u podru ju polarizacije elektroda jer oduzimanjem odgovarajueg CNaCl kanimo ukloniti upravo polarizaciju elektroda. Kapacitet bi na visokim frekvencijama trebao biti jednak i za lateks i za referentnu otopinu pa bi Ccorr=0. Meutim, to nije slu aj jer kapljice lateksa i referentne otopine nisu savraeno istih volumena. Kako se radi o 0,3-0,5% volumena kapljice  EMBED Equation.DSMT4 , neuklonjeni kapacitet smatramo aditivnom korekcijom i pretvaramo ga u  EMBED Equation.DSMT4 koji uvodimo u prilagodbu kao slobodni parametar na na in opisan u podpoglavlju 3.4. Porijeklo Gcorr je u tome ato G za referentnu otopinu biramo iz tablice, te nije mogue savraeno poklopiti tabli nu vodljivost sa onom od lateksa.  Slika 4.2: Frekventna ovisnost realnog dijela vodljivosti i kapaciteta Ca lateksa 210 nm nakon oduzimanja pozadine. Uo imo neuklonjeni dio vodljivosti Gcorr i kapaciteta Ccorr. Dobiveni podaci transformiraju se u realnu i imaginarnu komponentu dielektri ne funkcije pomou izraza (3.32) i (3.33) gdje je  EMBED Equation.DSMT4  u (3.32) i  EMBED Equation.DSMT4  u (3.33). Rezultat je prikazan na slici 4.3. U daljnjem tekstu, doprinose dielektri noj funkciji lateksa koje smo do sada ozna avali  EMBED Equation.DSMT4 i  EMBED Equation.DSMT4 radi jednostavnosti ozna avat emo  EMBED Equation.DSMT4 i  EMBED Equation.DSMT4 . Iz oblika krivulja vidimo dva moda, te se podaci dobiveni pomou izraza (3.32) i (3.33) prilagoavaju na HN funkciju za 2 moda pomou izraza (3.34) i (3.35). Prilikom prilagodbe rezultata va~no je odrediti granice prilagodbe, dakle, eksperimentalne podatke koji se uzimaju u obzir. Iako Gcorr izgleda dobro definiran (gornji dio slike 4.2), dobar izbor Gcorr potvruje se simetri noau zvonolikog oblika niskofrekventnog (NF) moda (gornji dio slike 4.3).  Slika 4.3: Frekventna ovisnost imaginarnog ( EMBED Equation.DSMT4 ) i realnog ( EMBED Equation.DSMT4 ) dijela doprinosa dielektri noj funkciji uzorka Ca lateksa 210 nm. Pune linije prikazuju rezultate prilagodbe na HN funkciju za dva moda, dok crtkane linije prikazuju niskofrekventni i visokofrekventni mod zasebno. Dobiveni parametri prilagodbe su navedeni u tablici 4.6. Slike 4.4a i 4.4b prikazuju zavranu kontrolu uspjeanosti prilagodbe. Na slici 4.4a je tzv. Cole- Cole graf koji pokazuje ovisnost imaginarnog i realnog dijela dielektri ne funkcije. Svaki mod predstavljen je jednim lukom kru~nice. Na slici 4.4b prikazana je frekventna ovisnost  EMBED Equation.DSMT4 Ca lateksa 210 nm nakon uklanjanja pozadine (puna linija). Pomou izraza 3.35, u kojeg uvrstimo prilagodbom dobivene parametre, dobijemo simuliranu Gsim() (crtkana linija) te provjerimo da li se poklapa sa eksperimentalnom Gexp.  a) b) Slike 4.4a i b: a)Cole- Cole graf dielektri nog odgovora dijaliziranog lateksa 210 nm. Pune linije prikazuju rezultate prilagodbe na HN funkciju za dva moda, dok crtkane linije prikazuju niskofrekventni i visokofrekventni mod zasebno predstavljen po jednim lukom kru~nice. Dobiveni parametri prilagodbe su navedeni u tablici 4.6. Va~an kriterij uspjeanosti je da to ke na desnom kraju (niske frekvencije) prate pune linije. Odsje ak na x- osi predstavlja ukupni doprinos lateksa dielektri noj konstanti uzorka. b) usporedba frekventne ovisnosti eksperimentalne i simulirane G() . Odstupanja se javljaju samo na najviaim frekvencijama jer u ovom prikazu naglaaavamo utjecaj parazitskih impenancija. Na prikazani na in obraeni rezultati mjerenja za latekse promjera estica 56 nm, 210 nm, 400 nm i 1000 nm (prije i nakon dijalize) prikazani su na slici 4.5. Naaa mjerenja pokazala su postojanje niskofrekventnog moda (u kHz frekventnom podru ju) i visokofrekventnog moda (u MHz frekventnom podru ju).  Slika 4.5: Frekventna ovisnost realnog i imaginarnog dijela doprinosa dielektri noj funkciji otopine lateksa (razli itih promjera). Pune linije prikazuju rezultate prilagodbe na HN funkciju za dva moda, dok crtkane linije prikazuju niskofrekventni i visokofrekventni mod zasebno. 5. DISKUSIJA Uo ene su dvije razli ite dielektri ne relaksacije. Primijetili smo i analizirali niskofrekventni mod (NF mod, frekventni opseg: od EMBED Equation.DSMT4 4kHz do EMBED Equation.DSMT4 0,5MHz) i visokofrekventni mod (VF mod, frekventni opseg: od EMBED Equation.DSMT4 2MHz do EMBED Equation.DSMT4 14MHz). Parametri prilagodbe (podpoglavlje 3.4) dani su u tablici 4.6. Osim jakosti dielektri ne relaksacije prikazano je i karakteristi no vrijeme relaksacije i iz njega izvedena karakteristi na duljina relaksacije. polistirenski lateks Interfacial Dynamics Co., SADNa+ Na+nedijalizirani Na lateksDeNFtNF (mS)LNF (nm)DeVFtVF (ns)LVF (nm)56180,32018114210994,3761043840020614,21374,3911110001119,21107,5539dijalizirani Ca lateksCa2+Ca2+56602,96620,513,54,5210954,1787,757,39,340026813,11402,742,57,9100045838,12391,668,510,1Tablica 4.6: Parametri prilagodbe na HN funkciju (podpoglavlje 3.2) dielektri nih doprinosa protuionske atmosfere lateksa, za latekse prije i nakon dijalize. DeNF je jakost dielektri ne relaksacije niskofrekventnog moda, tNF karakteristi no vrijeme relaksacije niskofrekventnog moda, LNF karakteristi na duljina relaksacije niskofrekventnog moda, DeVF je jakost dielektri ne relaksacije visokofrekventnog moda, tVF karakteristi no vrijeme relaksacije visokofrekventnog moda, LVF karakteristi na duljina relaksacije visokofrekventnog moda. Za nedijalizirani lateks kod ra unanja LNF i LVF ra unali smo sa difuzijskom konstantom za Na+ , a za dijalizirani lateks sa difuzijskom konstantom za Ca2+. Uslijed primjene stati kog elektri nog polja neka po etna koncentracija estica (u trenutku t=0 nalazi se u ishodiatu x=0) se difuzijom proairi. Srednji kvadrat pomaka dan je Einstein- Smoluchowski jednad~bom (1905):  EMBED Equation.DSMT4  gdje je  EMBED Equation.DSMT4  srednji kvadrat pomaka sferne estice u funkciji vremena, D difuzijska konstanta, t je vrijeme. Protuioni u atmosferi lateksa osciliraju i pri tome se gibaju difuznim mehanizmom. Kada se primjeni neko promjenjivo elektri no polje, za njihove pomake je uspostavljena veza izmeu karakteristi ne relaksacijske duljine i vremena relaksacije:  EMBED Equation.3  . Meutim, pitanje je koji ioni su relaksirajui te samim time sa kojom difuzijskom konstantom ra unamo:  EMBED Equation.DSMT4 ? Na temelju elementarne analize pretpostavit emo da su to veinski ioni. Dakle, u nedijaliziranom lateksu to su ioni Na+, a u dijaliziranom lateksu to su ioni Ca2+ . O'Brien  EMBED Equation.3  je teorijski pretpostavio postojanje dvije razli ite relaksacijske skale, tj. dva dielektri na moda. Vanjsko promjenjivo elektri no polje uzrokuje oscilacije protuionske atmosfere (slika 4.6a i b). Oscilacije se odvijaju du~ dvije karakteristi ne duljine: Debyeve duljine ( EMBED Equation.3 , okomito na povrainu estice) i dimenzije estice (2R, tj. du~ estice).  SHAPE \* MERGEFORMAT   SHAPE \* MERGEFORMAT  a) b) Slika 4.6a i b: a) nakon uklju ivanja vanjskog elektri nog polja dolazi do inicijalne preraspodjele naboja unutar difuzijskog sloja (na Debyevoj skali  EMBED Equation.DSMT4 ). b) nakon viae vremena dolazi do preraspodjele na skali promjera estica. Niskofrekventni mod (NF mod) Prvenstveni naa rezultat dobiven mjerenjem je ovisnost relaksacijskog vremena  EMBED Equation.3 NF o dimenziji estica 2R(slika 4.7a),  EMBED Equation.DSMT4 . Naa rezultat za NF mod je u skladu sa Schwanovim opa~anjima  EMBED Equation.3  koji je pronaaao 1 dielektri ni mod, radei u frekventnom opsegu 2- 200 kHz, te pokazao da relaksacijsko vrijeme raste sa (2R)2 (slika 4.7b)  b) Slika 4.7a i b: a) Ovisnost relaksacijskog vremena niskofrekventnog moda  EMBED Equation.DSMT4  o promjerima lateksa 2R. Puna linija prikazuje prilagodbu podataka na  EMBED Equation.DSMT4 . b) Ovisnost relaksacijskog vremena  EMBED Equation.DSMT4 o promjerima 2R prema Schwannu. Slika 4.8 prikazuje vezu karakteristi ne duljine na kojoj se odvija relaksacija LNF i promjera estica 2R. Kao ato slika prikazuje, LNF i 2R su proporcionalni ato je o ekivano jer je  EMBED Equation.DSMT4 , a kako smo pokazali da je  EMBED Equation.DSMT4  slijedi:  EMBED Equation.DSMT4 . Faktor proporcionalnosti koji dobivamo prilagodbom (puna linija) u izrazu  EMBED Equation.DSMT4  je 2,5. Isti faktor proporcionalnosti je uo en i u rezultatima mjerenja dielektri ne relaksacije vodenih otopina DNK molekula  EMBED Equation.DSMT4 . Zaklju ujemo da je NF mod koji smo uo ili posljedica relaksacije na skali  EMBED Equation.DSMT4  (slika 4.6b). Primjetimo da za dijalizirani lateks 56 nm, polo~aj NF moda odstupa od rezultata dobivenih za nedijalizirani lateks kao i od same teorijske linije (slika 4.7a). Za jakost NF moda ustanovili smo da linearno ovisi o dimenzijama estice (2R), a ne ovisi o koncentraciji iona i gustoi karboksilnih skupina  EMBED Equation.DSMT4  na povraini kuglice.  Slika 4.8: Ovisnost karakteristi ne duljine relaksacije niskofrekventnog moda LNF o promjerima lateksa 2R. Puna linija prikazuje prilagodbu podataka na izraz  EMBED Equation.DSMT4 . Crtkana linija prikazuje korespondenciju LNF=2R. Teorija jakosti odziva mo~e se razumjeti na sljedei jednostavan na in. Openito,  EMBED Equation.DSMT4  gdje je cef efektivna koncentracija protuiona, a  EMBED Equation.DSMT4  je polarizabilnost sistema, proporcionalna kvadratu karakteristi ne duljine relaksacije. Kao ato smo vidjeli na slici 4.8., karakteristi na duljina relaksacije direktno korelira sa promjerom estice pa imamo:  EMBED Equation.DSMT4 . No, mo~emo pretpostaviti da je efektivna koncentracija protuiona o kojoj se govori regulirana efektivnom povrainskom gustoom naboja jer je NF relaksacija ona u kojoj naboji osciliraju uz povrainu estice. Dakle, lateks ima specificiranu gustou  EMBED Equation.DSMT4  grupa na povraini (podpoglavlje 4.1). Efektivna povrainska gustoa naboja je, meutim, puno manja (dio grupa nije disociran, a dio je zasjenjen. Naime, u poglavlju 2, vidjeli smo da je povrainski potencijal  EMBED Equation.DSMT4 konstantan ( EMBED Equation.DSMT4 ) za stabilne koloide. Za sferi ne estice lateksa to zna i da je efektivni naboj Qef na povraini proporcionalan 2R jer je EMBED Equation.DSMT4 . Tada je povrainska gustoa  EMBED Equation.DSMT4 . Kako su kuglice lateksa u osnovi neutralne (svaka karboksilna skupina je neutralizirana jednim protuionom), to je gustoa protuiona cef koji sudjeluju u relaksaciji proporcionalna efektivnoj povrainskoj gustoi  EMBED Equation.DSMT4 . Uvrstimo li  EMBED Equation.DSMT4 i  EMBED Equation.DSMT4  u jednad~bu  EMBED Equation.DSMT4  , dobivamo  EMBED Equation.DSMT4 . Zaista, vidimo iz slike 4.9a da je  EMBED Equation.DSMT4  tj. iz slike 4.9b da je  EMBED Equation.DSMT4  . Ovo je joa jedna potvrda da protuionska atmosfera koja se nalazi u blizini povraine kuglice oscilira u vanjskom elektri nom polju ato mi detektiramo kao NF relaksacijski mod.  a) b) Slika 4.9: a) ovisnost jakosti dielektri ne relaksacije niskofrekventnog moda EMBED Equation.DSMT4  o promjerima lateksa 2R. Puna linija prikazuje prilagodbu podataka na izraz  EMBED Equation.DSMT4  b) ovisnost  EMBED Equation.DSMT4  o promjerima lateksa 2R. Puna linija prikazuje prilagodbu podataka na izraz EMBED Equation.DSMT4 . Visokofrekventni mod (VF mod) Prema teorijskom modelu O'Briena, visokofrekventni mod se treba odvijati na skali Debyeve duljine (korelirana sa ionskom vodljivosti slobodnih nosioca, podpoglavlje 2.1). Prema elementarnoj analizi vidjeli smo da je red veli ine koncentracije protuiona Na+ ili Ca2+ oko 1 mM (podpoglavlje 4.2). Kako se Debyeva duljina ra una iz koncentracije iona (izraz 2.8), Debyeva duljina u naaim lateksima je reda 10 nm. Kao ato vidimo u tablici 4.6, za naae latekse LVF su reda 10 nm tj. korelacija je primjetna. Taj rezultat je, dakle, takoer u skladu s O'Brienovim modelom. Na slici 4.10 je prikazana dielektri na jakost VF moda u ovisnosti o 2R. Vidimo da  EMBED Equation.DSMT4  opada sa  EMBED Equation.DSMT4 . Budui smo uzeli da je LVF podjednak za sve latekse (LVF= konst.), to bi i  EMBED Equation.DSMT4  tj. efektivna koncentracija protuiona koji sudjeluju u VF relaksaciji bila isto proporcionalna sa  EMBED Equation.DSMT4 . Dakle, i za VF relaksaciju, efektivna koncentracija protuiona je odreena povrainskom gustoom naboja na kuglici koja za naae latekse ovisi kao  EMBED Equation.DSMT4 . Time je potvreno da je i VF relaksacija u lateksu ovisna o koncentraciji iona u atmosferi lateks kuglica, a ne o koncentraciji slobodnih iona u bulk otopini.  Slika 4.10: Ovisnost jakosti dielektri ne relaksacije visokofrekventnog moda  EMBED Equation.DSMT4  o promjerima lateksa 2R. Puna linija prikazuje prilagodbu podataka na izraz  EMBED Equation.DSMT4 . 6. ZAKLJU AK U ovom radu prikazali smo modele elektri nog dvosloja (nastaje kao posljedica akumulacije naboja uz povrainu elektroda) te uz elektri ni dvosloj vezan efekt polarizacije elektroda. Opisali smo odreivanje dielektri ne funkcije mjerenjem kompleksne admitancije niskofrekventnom dielektri nom spektroskopijom te na in obrade dobivenih podataka na primjeru polistirenskih lateksa (netretiranih i dijaliziranih). Utvrdili smo da metoda oduzimanja pozadine dobro funkcionira na primjeru istra~ivanih lateksa (monodisperzni polistirenski lateksi dimenzija estica: 56 nm, 210 nm, 400 nm i 1000 nm). Sukladno teorijskim o ekivanjima potvrdili smo postojanje dva dielektri na moda te sukladno tome analizirali niskofrekventnu i visokofrekventnu dielektri nu relaksaciju. Dielektri ni odgovor lateksa prilagoen je zbroju dvije HN funkcije. Niskofrekventni mod povezan je sa relaksacijom na skali promjera lateksa. Visokofrekventni mod mo~e se pripisati relaksacijama na skali Debyeve duljine. BIBLIOGRAFIJA  EMBED Equation.DSMT4  R. J. Hunter, Foundations of Colloid Science, Oxford University Press Inc., New York 2001.  EMBED Equation.DSMT4  S. Takashima, Dielectric dispersion of deoxyribonucleic acid, J. Phys. Chem. 70(5), 1372- 1379, 1966.  EMBED Equation.DSMT4  K.Radmanovi, Komora za mjerenje dielektri ne konstante uzoraka u tekuoj fazi, diplomski rad, Prirodoslovno- matemati ki fakultet Sveu iliata u Zagrebu, 2006.  EMBED Equation.DSMT4  C. Grosse, M. Tirado, W. Pieper i R. Pottel, J. Colloid Interface Sci. 205, 26-41 (1998) i M. Pinteri, T. Vuleti, M. Lon ari, S. Tomi i J. U. von Schutz, Low frequency dielectric spectroscopy of the Peierls- Mott insulating state in the deuterated copper- DCNQI systems, Eur. Phys. J. B16, 487-493 (2000).  EMBED Equation.DSMT4  F. Bordi, C. Cametti i R.H. Colby, J. Phys.: Condens.Matter 16, R1423-1463 (2004) i B. Saif, R.K. Mohr, C.J. Montrose, and T.A. Litovitz, Biopolymers 31, 1171-1180 (1991).  EMBED Equation.DSMT4  S. Havriliak i S. Negami, J. Polym. Sci. C 14, 99-117 (1966).  EMBED Equation.DSMT4  H. Haruta, The Impedance Measurement Handbook, 2nd edition (Agilent Technologies, USA/Japan, 2000).  EMBED Equation.DSMT4  Interfacial Dynamics Corporation, Certificate of Analysis.  EMBED Equation.DSMT4  B. Frka-Peteai, Utilisation de la spectroscopie dielectrique basse frequence dans l' etude de systemes collodaux, seminarski rad, Institut za fiziku i Universit Denis Diderot Paris VII, 2005.  EMBED Equation.DSMT4  P. W. Atkins, M. J. Clugston, Na ela fizikalne kemije, `kolska knjiga, Zagreb 1990.  EMBED Equation.DSMT4  R. W. O' Brien, J. Coll. Interface Sci 113, 81-93 (1986).  EMBED Equation.DSMT4  H. P. Schwann, G. Schwarz, J. Maczuk i H. Pauly, J. Phys. Chem. 66, 2626-2635 (1962).  EMBED Equation.DSMT4  S. Tomi, T. Vuleti, S. Dolanski Babi, S. Kr a, D. Ivankovi, L. Gripari, R. Podgornik, Phys. Rev. Lett 97, 098303  EMBED Equation.DSMT4  (2006) i S. Tomi, S. Dolanski Babi, T. Vuleti, S. Kr a, D. Ivankovi, L. Gripari, R. Podgornik, Dielectric relaxation of DNA aqueous solutions, cond-mat/0602255  EMBED Equation.DSMT4 . DODATAK A) FIZIKALNE VELI INE Fizikalna veli inaOznakaJedinica(specifi na) kompleksna vodljivosts(w)1/(Wm)Boltzmannova konstantakB1,38 EMBED Equation.DSMT4 10-23 J/Kdielektri na funkcijae(w)bez dimenzijadielektri na konstanta vodeeH2079,38 na T=298,15 K dielektri ni pomakDC/m2difuzijska konstantaDm2/sdipolni momentpCmdruga derivacija koordinate po vremenu EMBED Equation.DSMT4 m/s2efektivna masam*kgelektri no poljeEV/melektrostatski potencijal EMBED Equation.DSMT4 Vgustoa strujejA/m2imaginarni dio dielektri ne funkcijee''(w)bez dimenzijaimaginarni dio kompleksne admitancijeB(w)1/WimpedancijaZWionska jakost elektrolitaImol/Ljakost relaksacijskog procesaDebez dimenzijakapacitetCFkarakteristi no vrijeme relaksacijet0skompleksna admitancijaY(w)1/Wkoncentracijacmol/Lkonstanta disocijacijeKamol/Lkonstanta elasti nostikkg/s2konstanta guaenjagkg/skonstanta komoreKm-1koordinataxmkru~na frekvencija w1/smagnetsko poljeHTmolarna vodljivost EMBED Equation.DSMT4  EMBED Equation.DSMT4 S/cm/ EMBED Equation.DSMT4 MnabojQCnaboj elektronae1,6 EMBED Equation.DSMT4 10-19 CotporR EMBED Equation.DSMT4 permitivnost vakuumae08,858 EMBED Equation.DSMT4 10-12 F/mpolarizabilnost EMBED Equation.DSMT4 C2m2/Jpolarizacija P(w)C/m2povrainaSm2povrainska gustoa naboja EMBED Equation.DSMT4 C/m2promjer estice2Rnmprva derivacija koordinate po vremenu  EMBED Equation.DSMT4 m/srazlika naponaUVrealni dio dielektri ne funkcijee'(w)bez dimenzijarealni dio kompleksne admitancijeG(w)1/Wrelativna permitivnost elektrolita EMBED Equation.DSMT4 bez dimenzijastrujaIAsvojstvena frekvencija titranja materijalaw01/stemperaturaTKvanjsko elektri no poljeE(w)V/mvolumna gustoa nabojarC/m3vremenska konstanta guaenjats B) KAZALO POJMOVA Bandwidth (BW)- postavka na Agilent ureaju koja omoguava brzo mjerenje jedne to ke, tj. jednog spektra. bulk otopina- dio otopine u kojem je raspodjela protuiona i koiona homogena. Debyeva duljina- udaljenost na kojoj se potencijal smanji za 1/e od njegove vrijednosti na povraini metala. Definira se i kao mjera airine dvosloja. difuzni dvosloj- dio otopine, koji se prote~e od vanjske Helmholtzove ravnine do bulk otopine, u kojem se koncentracija protuiona smanjuje sa udaljenoau od povraine. dijaliza- odvajenje otopljenih tvari iz koloidne otopine pomou membrana vrlo finih pora. Kroz takve membrane prolaze ioni, a zaostaju estice koloidnih dimenzija. elektri ni dvosloj- nastaje akumulacijom naboja iz otopine uz suprotno nabijenu povrainu elektrode. elektrolit- tvar koja rastaljena ili otopljena u vodi provodi elektri nu struju. Taljenjem ili otapanjem disocira na elektri ki nabijene estice (ione). fenilna skupina- funkcionalna skupina ija je formula C6H5. 6 atoma ugljika cikli ki je povezano u aromatski prsten. karboksilna skupina- funkcionalna skupina koja je zajedni ka svim karboksilnim kiselinama. koioni- ioni jednakog naboja kao i povraina elektrode. koloidne estice- grubo se definiraju kao estice ija je linearna dimenzija u rasponu 10- 1000 nm. koloidne disperzije- otopine u kojima su molekule otopljene tvari, disperzirane u otapalu, mnogo vee od molekula otapala. lateks- organski polimer (mlije ni sok nekih tropskih biljaka) koji sadr~i kuglice ije su dimenzije usporedive sa valnom duljinom svjetlosti pa rasprauju svjetlost na sve strane te je zato lateks mlije nog izgleda. Peltierovi elementi- poluvodi ki elementi koji rade kao toplinske pumpe i slu~e za grijanje/hlaenje komore. pH- negativni logaritam koncentracije vodikovih iona. pKa- negativni logaritam konstante disocijacije. polistireni- vinilni polimeri koji se dobivaju iz monomera stirena. Strukturno, polistiren je dugi ugljikovodikov lanac s fenilnom skupinom vezanom na svaki drugi ugljikov atom. protuioni- ioni suprotnog naboja od naboja povraine elektrode. ravnina posmaka- granica Sternovog sloja i difuznog sloja. titracija- metoda koja se temelji na neutralizaciji kiseline ili baze nepoznate koncentracije sa bazom ili kiselinom poznate koncentracije. unutraanja Helmholtzova ravnina (UHR)- dio Sternovog sloja koji se definira kao srediate specifi no adsorbiranih iona. vanjska Helmholtzova ravnina (VHR)- definiraju ju ioni koji nisu izgubili omota  otapala (hidratacijsku ovojnicu). zeta potencijal- elektri ni potencijal na granici Sternovog sloja i difuznog sloja. C) METODI KI DIO Utjecaj dielektri nog sredstva na kapacitet kapacitora Uvod Nastavna tema  Utjecaj dielektri nog sredstva na kapacitet kapacitora obrauje se unutar cjeline  Elektri ne i magnetne pojave u drugom razredu gimnazije i predviena je za jedan nastavni sat. Priprema za nastavu Nastavna jedinica: Elektri ni kapacitet, elektri ni kapacitor. Odgojno- obrazovni cilj: Rjeaavanjem problemske situacije odrediti utjecaj dielektri nog sredstva na kapacitet kapacitora, uvoenje pojma relativne permitivnost sredstva, izraza za kapacitet ravnog kapacitora s dielektrikom, poopenje Coulombovog zakona, elektri nog polja i elektri nog potencijala to kastog naboja u slu ajevima kada naboji nisu u vakuumu nego u dielektri nom sredstvu, mikroskopsko tuma enje dielektri nosti. Oblici rada: Interaktivni oblik nastave temeljen na konstruktivisti kom pristupu. Nastavna sredstva: Pribor za pokus, Power point prezentacija, plo a. Razrada sata Kao uvodno pitanje za u enike mo~e se postaviti problem koji omoguuje divergentno razmialjanje u enika. Iako u enici o tome nemaju relevantnog predznanja (nisu joa uli o relativnoj permitivnosti sredstva), ipak bi moglo biti zanimljivo vidjeti njihove eventualne ideje. Jedna od konstruktivnih ideja bi bila da se to mo~e razrijeaiti pokusom. Problem: prostor izmeu plo a ravnog kapacitora sasvim ispunimo nekim izolatorom (npr. staklom). Kako e se to odraziti na kapacitet kapacitora? Hoe li se time kapacitet C smanjiti, poveati, ili ostati isti? Kako u izolatoru nema slobodnih nosioca naboja, u enici mogu pomisliti da se niata ne bi trebalo promijeniti, tj. da bi C trebao ostati isti. Meutim, to nije to no ato se najbolje mo~e pokazati pokusom. U enicima se poka~e pribor pripremljen za izvedbu pokusa. Pitanje za u enike: Kakav bi se pokus mogao izvesti tim priborom da bi se dobio odgovor na uvodno pitanje? Pokus se izvede nakon ato se u raspravi zaklju i kakav pokus treba izvesti. Pokus: dvije u vraene metalne plo e ine kapacitor. Jednu spojimo na elektroskop, a drugu uzemljimo (slika C.1). Potencijal Zemlje po dogovoru je V=0. Na prvu plo u dovedemo naboj +Q ime se na drugoj plo i influencira naboj  Q. Naboji su uniformno rasporeeni du~ unutraanjih povraina plo a uzrokujui tako povrainsku gustou naboja  EMBED Equation.DSMT4  gdje je S povraina plo e kapacitora . Plo e kapacitora su na razli itim potencijalima, a razlika potencijala jednaka je naponu kapacitora U. Jakost elektri nog polja izmeu plo a u vakuumu je:  EMBED Equation.DSMT4 . Razlika potencijala (rad po jedini nom naboju potreban za prenoaenje malog naboja sa jedne plo e na drugu):  EMBED Equation.DSMT4  gdje je l razmak izmeu plo a kapacitora. Napon je proporcionalan naboju, a koeficijent proporcionalnosti C (kapacitet) za razmatrani sustav od dviju plo a u vakuumu jednak je:  EMBED Equation.DSMT4  tj. vrijedi relacija  EMBED Equation.DSMT4 . Naboj +Q ostaje u pokusu nepromijenjen jer je ta plo a, zajedno s elektroskopom na koji je priklju ena, izolirana od okoline. Iz relacije  EMBED Equation.DSMT4  slijedi da e otklon listia elektroskopa (koji je proporcionalan s  EMBED Equation.DSMT4 ) biti to manji ato je kapacitet vei. Na po etku, kad je izmeu plo a zrak (zrak se kao izolator ponaaa vrlo sli no vakuumu), zabilje~imo otklon elektroskopa. Zatim izmeu plo a kapacitora stavimo npr. staklo te zabilje~imo otklon elektroskopa. Pokus mo~emo ponoviti tako da umjesto stakla stavimo neki drugi izolator. Jasno se moraju vidjeti rezultati opa~anja, tj. da se umetanjem dielektrika izmeu plo a kapacitora otklon listia smanjio.  EMBED Visio.Drawing.11  Slika C.1: Pokus: Utjecaj dielektri nog sredstva na kapacitet kapacitora. Sljedee pitanje na koje u enici moraju nai odgovor: Zna i li smanjivanje otklona listia elektroskopa u izvedenom pokusu poveanje ili smanjivanje kapaciteta? Rasprava zavraava uvoenjem novog pojma, relativne permitivnosti sredstva, i izrazom za kapacitet ravnog kapacitora sa dielektrikom:  EMBED Equation.DSMT4 . U enicima se navedu vrijednosti relativne permitivnosti za neke materijale kako bi stekli dojam o redu veli ine od  EMBED Equation.DSMT4 . Posebno treba upamtiti vrijednosti za vakuum (1,00000) i zrak (1,00054) da bi se shvatilo kako je ta razlika neznatna, te za vodu (7,8) koja ima veliku relativnu permitivnost. Uvoenjem relativne permitivnosti potrebno je poopiti Coulombov zakon i na slu ajeva kad naboji nisu u vakuumu nego u dielektri nom sredstvu relativne permitivnosti  EMBED Equation.DSMT4 . Konstanta  EMBED Equation.DSMT4  ve se pojavljivala u mnogim razmatranjima, npr. u izrazu za Coulombov zakon, u konstanti  EMBED Equation.DSMT4 . To upuuje na injenicu da smo te pojave razmatrali u vakuumu. Razmatramo li iste pojave u nekom dielektri nom sredstvu, tada se permitivnost dielektrika poveava  EMBED Equation.DSMT4  puta te se umjesto  EMBED Equation.DSMT4  pojavljuje umno~ak  EMBED Equation.DSMT4 . Isto bi trebalo u initi za elektri no polje i elektri ni potencijal to kastog naboja. Od u enika treba zahtijevati da to poopenje na ine sami. Kvalitativan rezultat izvedenog pokusa je: izolator (ili dielektri no sredstvo) poveava kapacitet kapacitora. Kvantitativna ispitivanja pomou preciznijih metoda pokazuju da odreeni dielektrik poveava kapacitet kapacitora za faktor  EMBED Equation.DSMT4  koji se zove relativna permitivnost tog dielektrika. Faktor  EMBED Equation.DSMT4  je isti broj koji pokazuje koliko je puta permitivnost konkretnog materijala (dielektrika) vea od permitivnosti vakuuma  EMBED Equation.DSMT4 . Dakle, vrijedi:  EMBED Equation.DSMT4 . Va~no svojstvo dielektrika je i elektri no polje proboja  EMBED Equation.DSMT4 . To je ona vrijednost elektri nog polja u dielektriku na kojoj dolazi do elektri nog proboja, tj. dielektrik postaje vodljiv i time gubi dielektri na svojstva. U elektrotehnici se upotrebljavaju razli iti tipovi kapacitora, ali svi uz uporabu nekog dielektrika koji im poveava kapacitet u skladu sa relacijom:  EMBED Equation.DSMT4 . U skladu sa tom relacijom po~eljno je da povraina  EMBED Equation.DSMT4  bude ato vea, a razmak l ato manji. Kapacitor u elektroni kim krugovima slu~i kao  skladiate naboja. Dakle, apsorbira ili isporu uje naboj. U elektroni kim instrumentima i kompjuterima pomou kapacitora mo~e se dobiti odreena promjena napona kao posljedica odreene promjene naboja. Mikroskopsko tuma enje dielektri nosti Uvoenjem parametra  EMBED Equation.DSMT4  opisali smo utjecaj dielektrika samo pojavno, tj. naali smo zakonitost koja nam omoguuje da za zadanu situaciju predvidimo kakav e biti utjecaj dielektrika. No takav makroskopski pristup na mo~e objasniti zaato dielektrici pokazuju baa takva svojstva. Objaanjenje dielektri nosti mo~e se potra~iti jedino u sklopu mikroskopskog modela tvari. Za objaanjenje navedenog ponaaanja dielektrika valja razmotriti ato se zbiva u dielektriku na mikroskopskoj ljestvici. Dakle, valja razmotriti koja to posebna svojstva molekula dielektri nog materijala uzrokuju njihovo opa~eno, tj. makroskopsko ponaaanje. Razlog je u tome ato su molekule dielektrika elektri ni dipoli: ukupni naboj molekule jest nula, ali su pozitivni i negativni naboji unutar molekule meusobno malo razmaknuti. Molekula ima na jednoj strani viaak pozitivnog, a na drugoj viaak negativnog naboja. Zbog toga molekula elektri ki meudjeluje s neposrednim okoliaem (na mikroskopskim udaljenostima), a i sa vanjskim elektri nim poljem. Mogue je da su u enici neke pojmove (nesimetri an raspored naboja u molekuli, molekule kao elektri ni dipoli) ve uli u kemiji, pa bi to trebalo ve na po etku utvrditi pitanjima za u enike i raspravom. U vanjskom elektri nom polju takve se molekule zakreu tako da budu orijentirane du~ silnica elektri nog polja. Ta se pojava zove polarizacija dielektrika. Dakle, dielektrik je elektri ki neutralan, ali dolazi do redistribucije pozitivnih i negativnih naboja unutar dielektrika te uslijed toga do induciranja naboja na povraini dielektrika. Ukupni u inak polarizacije dielektrika u vanjskom elektri nom polju jest da svojim doprinosom umanjuje ukupno elektri no polje unutar dielektrika (slika C.2a i b).  EMBED Visio.Drawing.11  EMBED Visio.Drawing.11  Slika C.2a i b:a) Linije elektri nog polja kada je izmeu plo a kondenzatora vakuum.b) Inducirani naboji u dielektriku smanjuju elektri no polje. Popis literature za metodi ki dio: 1) Rudolf Krsnik, Fizika 2, `kolska knjiga, Zagreb, 1997. 2) Rudolf Krsnik, Metodi ki priru nik za nastavnike: fizika 2, `kolska knjiga, Zagreb, 2003. 3) Hugh D. Young , Roger A. Freedman, Sears and Zemansky's univarsity physics: with modern physics- 11 th ed., Pearson Education Inc., 2004.     PAGE 1 PAGE 2  EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.3   EMBED Equation.3   EMBED Equation.3   EMBED Equation.3   EMBED Equation.3  kation okru~en molekulama vode specifi no adsorbirani anion adsorbirani sloj molekula vode metal UHR VHR difuzni sloj dehidratizirani anion hidratizirani anion hidratizirani kation bulk difuzni sloj UHR VHR h  EMBED Equation.DSMT4  dehidratizirani anion hidratizirani anion hidratizirani kation  EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.DSMT4   EMBED Equation.DSMT4  U+ - U-  EMBED Equation.DSMT4  U- U+  EMBED Equation.DSMT4   EMBED Equation.DSMT4  + + - - - tekui uzorci GHz-THz kHz-MHz 1 LCUR LPOT HPOT HCUR 2 1 metalno kuiate Pthg nbn CENTRALNI VOD OKLOP 3 Vs Is Zs Rso Vosc eHF=1  EMBED Equation.DSMT4  povrainska gustoa naboja  COO- skupina Na+ OH- lateks voda LVF  EMBED Equation.DSMT4  LNF EMBED Equation.DSMT4  Rdl1 Rdl2  EMBED Equation.DSMT4  de(()  EMBED SigmaPlotGraphicObject.4 Error! 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