ࡱ> M   {!!s""|##u$$s%%5@bjbj22 @XXt) P>P>P>?,,,x?rzl$4XX|EtGtGtGtGtGtGt$~R0DktP> {}&   ktX,z{{{ 4 &XP>Et{ Et{{~]8`/P>ft @),='/aX9l Bz0rzat|tf"??tP>9f  {     ktkt??ZD_?? SVEU ILI`TE U ZAGREBU PRIRODOSLOVNO  MATEMATI KI FAKULTET  DIPLOMSKI RAD PRIPRAVA I IDENTIFIKACIJA POLIOKSOMOLIBDATA VESNA CMRE KI Zagreb, 2005. VESNA CMRE KI Priprava i identifikacija polioksomolibdata DIPLOMSKI RAD Predlo~en Kemijskom odsjeku Prirodoslovno-matemati kog fakulteta Sveu iliata u Zagrebu radi stjecanja zvanja diplomirani in~enjer kemije Zagreb, o~ujak 2005. Ovaj diplomski rad izraen u Zavodu za opu i anorgansku kemiju Prirodoslovno-matemati kog fakulteta u okviru znanstvenog projekta  Sinteza i struktura kompleksa-katalizatora u kemijskim i bioloakim reakcijama , pod mentorstvom dr. sc. Marine Cindri te neposrednim vodstvom dr. sc. Vianje Vrdoljak, predan je na ocjenu Kemijskom odsjeku Prirodoslovno-matemati kog fakulteta Sveu iliata u Zagrebu radi stjecanja zvanja diplomirani in~enjer kemije. Dan odr~avanja diplomskog ispita odreen je za datum 16. o~ujka 2005., a povjerenstvo imenovano u sastavu: dr. sc. Vianja Vrdoljak, doc. ________________________ dr. sc. Davor Kova evi, doc. ________________________ dr. sc. Nives Gali, doc. ________________________ zamjena: dr. sc. Marina Cindr, izv. prof., ________________________ ocijenilo je ovaj diplomski rad ocjenom: ______________________. U Zagrebu, 16. o~ujak 2005. ZAHVALA  Iskreno se zahvaljujem dr. sc. Marini Cindri i dr. sc. Vianji Vrdoljak na savjetima, pomoi i vodstvu prilikom izrade ovog diplomskog rada. Zahvaljujem dr. sc. Zorici Veksli na pomoi i uputama prilikom karakterizacije produkata elektronskom paramagnetskom rezonancijom, dr. sc. Tanji Kajfe~ Novak na pomoi i uputama prilikom snimanja difraktograma praha te koriatenja CSD baze podataka te dr. sc. Ernestu Meatroviu, Ljubici Ljubi i Bo~eni Mandi. Takoer zahvaljujem svim ostalim lanovima zavoda koji su mi svjesno ili nesvjesno pomogli pri izradi ovog rada te u inili izradu diplomskog rada zanimljivom, veselom i uspjeanom. Velika hvala mami Ivanki, tati Zvonku i bratu Alenu na vjeri, podraci i bezuvjetnom povjerenju u mene koje ste mi pru~ili tijekom mog akolovanja. Zahvaljujem se Filipu Kova iu i Krunoslavu Mirosavljeviu na savjetima i podraci prilikom pisanja ovog rada. Vesna Cmre ki   U imo se sanjati, moja gospodo, jer tako emo vjerojatno nai istinu, ali uvajmo se objave naaih snova prije nego ih provjerimo budnim razumom. Friederich August Kekul,  Benzenska sve anost , 1890. g. Berlin. SADR}AJ  Temeljna dokumentacijska kartica Basic documentation card  TOC \o "1-1" \h \z \t "Heading 2;2;Heading 3;3"  HYPERLINK \l "_Toc98085545" 1. Uvod COMMENTS \* MERGEFORMAT   HYPERLINK \l "_Toc98085548" 1.1. Svrha rada  PAGEREF _Toc98085548 \h 1  HYPERLINK \l "_Toc98085549" 1.2. Povijesni pregled  PAGEREF _Toc98085549 \h 2  HYPERLINK \l "_Toc98085550" 2. Literaturni pregled COMMENTS \* MERGEFORMAT   HYPERLINK \l "_Toc98085552" 2.1. Strukturna svojstva polioksometalata  PAGEREF _Toc98085552 \h 4  HYPERLINK \l "_Toc98085553" 2.2. Fizikalno - kemijska svojstva polioksometalata  PAGEREF _Toc98085553 \h 8  HYPERLINK \l "_Toc98085554" 2.3. Polioksometalati molibdena(VI)  PAGEREF _Toc98085554 \h 10  HYPERLINK \l "_Toc98085555" 2.3.1. Derivati polioksomolibdata(VI) s aminokiselinama  PAGEREF _Toc98085555 \h 13  HYPERLINK \l "_Toc98085556" 2.3.2. Polioksoalkoksomolibdati(VI)  PAGEREF _Toc98085556 \h 16  HYPERLINK \l "_Toc98085557" 2.3.3. Fotokromizam polioksomolibdata(VI)  PAGEREF _Toc98085557 \h 17  HYPERLINK \l "_Toc98085558" 2.3.4. Velike klusterske strukture s polioksomolibdatnim jezgrama  PAGEREF _Toc98085558 \h 19  HYPERLINK \l "_Toc98085559" 3. Eksperimentalni dio COMMENTS \* MERGEFORMAT   HYPERLINK \l "_Toc98085562" 3.1. Priprava diklorodioksomolibdena(VI), MoO2Cl2  PAGEREF _Toc98085562 \h 24  HYPERLINK \l "_Toc98085563" 3.2. Reakcije diklorodioksomolibdena(VI) s aminokiselinama i morfolinom  PAGEREF _Toc98085563 \h 24  HYPERLINK \l "_Toc98085564" 3.2.1. Reakcije diklorodioksomolibdena(VI) s D,L-metioninom, D,L-alaninom, L-leucinom, L-valinom i morfolinom pri sobnoj temperaturi  PAGEREF _Toc98085564 \h 24  HYPERLINK \l "_Toc98085565" 3.2.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom, D,L-alaninom i morfolinom pri povienoj temperaturi  PAGEREF _Toc98085565 \h 25  HYPERLINK \l "_Toc98085566" 3.2.3. Prekristalizacija polioksomolibdata(VI) s D,L-metioninom i morfolinom iz vode  PAGEREF _Toc98085566 \h 26  HYPERLINK \l "_Toc98085567" 3.3. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom  PAGEREF _Toc98085567 \h 26  HYPERLINK \l "_Toc98085568" 3.3.1. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom pri sobnoj temperaturi  PAGEREF _Toc98085568 \h 26  HYPERLINK \l "_Toc98085569" 3.3.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom pri povienoj temperaturi  PAGEREF _Toc98085569 \h 27  HYPERLINK \l "_Toc98085570" 3.4. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i -pikolinom  PAGEREF _Toc98085570 \h 27  HYPERLINK \l "_Toc98085571" 3.4.1. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i g-pikolinom pri sobnoj temperaturi  PAGEREF _Toc98085571 \h 27  HYPERLINK \l "_Toc98085572" 3.4.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i g-pikolinom pri poviaenoj temperaturi  PAGEREF _Toc98085572 \h 28  HYPERLINK \l "_Toc98085573" 3.5. Reakcije diklorodioksomolibdena(VI) s organskim bazama: g-pikolinom, trietilaminom i morfolinom  PAGEREF _Toc98085573 \h 28  HYPERLINK \l "_Toc98085574" 3.5.1. Reakcija diklorodioksomolibdena(VI) s g-pikolinom pri sobnoj temperaturi  PAGEREF _Toc98085574 \h 28  HYPERLINK \l "_Toc98085575" 3.5.2. Reakcija diklorodioksomolibdena(VI) i trietilamina pri sobnoj temperaturi  PAGEREF _Toc98085575 \h 28  HYPERLINK \l "_Toc98085576" 3.5.3. Reakcija diklorodioksomolibdena(VI) i morfolina pri sobnoj temperaturi  PAGEREF _Toc98085576 \h 29  HYPERLINK \l "_Toc98085577" 3.5.4. Reakcija diklorodioksomolibdena(VI) i morfolina pri povienoj temperaturi  PAGEREF _Toc98085577 \h 29  HYPERLINK \l "_Toc98085578" 3.6. Metode identifikacije izoliranih produkata  PAGEREF _Toc98085578 \h 30  HYPERLINK \l "_Toc98085579" 3.6.1. Kemijska analiza sadr~aja molibdena  PAGEREF _Toc98085579 \h 30  HYPERLINK \l "_Toc98085580" 3.6.2. Kvalitativni test na kloride  PAGEREF _Toc98085580 \h 30  HYPERLINK \l "_Toc98085581" 3.6.3. Kemijska analiza sadr~aja ugljika, vodika i duaika  PAGEREF _Toc98085581 \h 31  HYPERLINK \l "_Toc98085582" 3.6.4. Termogravimetrijsko odreivanje sadr~aja molibdena  PAGEREF _Toc98085582 \h 31  HYPERLINK \l "_Toc98085583" 3.6.5. Infracrvena spektroskopija  PAGEREF _Toc98085583 \h 32  HYPERLINK \l "_Toc98085584" 3.6.6. UV-ozra ivanje  PAGEREF _Toc98085584 \h 32  HYPERLINK \l "_Toc98085585" 3.6.7. Elektronska paramagnetska rezonancija  PAGEREF _Toc98085585 \h 32  HYPERLINK \l "_Toc98085586" 3.6.8. Difrakcija rentgenskih zraka na polikristalnom uzorku  PAGEREF _Toc98085586 \h 33  HYPERLINK \l "_Toc98085587" 4. Rezultati i rasprava COMMENTS \* MERGEFORMAT   HYPERLINK \l "_Toc98085588" 4.1. Identifikacija morfolinijevih polioksomolibdata(VI)  PAGEREF _Toc98085588 \h 35  HYPERLINK \l "_Toc98085590" 4.2. Identifikacija trietilamonijevih polioksomolibdata(VI)  PAGEREF _Toc98085590 \h 39  HYPERLINK \l "_Toc98085592" 4.3. Identifikacija -pikolinskih polioksomolibdata(VI)  PAGEREF _Toc98085592 \h 41  HYPERLINK \l "_Toc98085593" 4.4. Identifikacija produkata infracrvenom spektroskopijom  PAGEREF _Toc98085593 \h 43  HYPERLINK \l "_Toc98085594" 4.5. Identifikacija produkata termogravimetrijskom i kemijskom analizom  PAGEREF _Toc98085594 \h 45  HYPERLINK \l "_Toc98085595" 5. Zaklju ak 47  HYPERLINK \l "_Toc98085596" 6. Literaturni izvori 48  HYPERLINK \l "_Toc98085597" 7. Kratice 50  HYPERLINK \l "_Toc98085598" 8. Dodatak 52  HYPERLINK \l "_Toc98085599" 9. }ivotopis 62  TEMELJNA DOKUMENTACIJSKA KARTICA Sveu iliate u Zagrebu Diplomski rad Prirodoslovno-matemati ki fakultet Kemijski odsjek PRIPRAVA I IDENTIFIKACIJA POLIOKSOMOLIBDATA VESNA CMRE KI Zavod za opu i anorgansku kemiju, Prirodoslovno-matemati ki fakultet, Sveu iliate u Zagrebu, Ulica kralja Zvonimira 8, 10 000 Zagreb, Republika Hrvatska SA}ETAK U ovom diplomskom radu ispitivane su reakcije diklorodioksomolibdena(VI) (MoO2Cl2) s D,L- metioninom, D,L- alaninom, L-leucinom i L-valinom, uz dodatak metanolne otopine morfolina ili trietilamina ili -pikolina. Sve reakcije izvedene su u metanolu: a) pri sobnoj temperaturi, b) uz refluks. Fotoosjetljivost reaktanata i produkata zahtijevala je izvoenje reakcija i uvanje kemikalija u mraku. Produkti su identificirani na osnovi podataka dobivenih infracrvenom spektroskopijom, termogravimetrijskom analizom, difrakcijom rentgenskih zraka na polikristalnom uzorku, elektronskom paramagnetskom rezonancijom nakon izlaganja UV-zra enju te kemijskom analizom. Produkti su identificirani kao polioksometoksomolibdati(VI), kod kojih je umjesto aminokiseline doalo do vezanja metokso (-OCH3) skupine na oktamolibdatnu jezgru. To se mo~e protuma iti nestabilnoau i osjetljivoau takvih spojeva. Zaklju eno je da reakcijski uvjeti bitno utje u na strukturu i sastav izoliranih produkata. Izolirani i identificirani su sljedei produkti: [C4H10NO]6[Mo8O26(OCH3)2], [C4H10NO]4[Mo8O26]2H2O, [C4H10NO]4[Mo8O24(OCH3)4], [C6H8N]4[Mo8O24(OCH3)4], [C6H8N]4[Mo8O24(OCH3)4]3CH3OH, trietilamonijev oktamolibdat i [Et3NH]2[MoO4]. Rad sadr~i: 61 stranicu, 29 slika, 38 literaturnih navoda, 4 tablice i napisan je na hrvatskom jeziku. Pohranjen je u knji~nici Zavoda za opu i anorgansku kemiju Prirodoslovno-matemati kog fakulteta, Sveu iliata u Zagrebu. Klju ne rije i: molibden(VI), polioksometalati Mo(VI), aminokiseline, oktamolibdat, polioksoalkoksomolibdati. Mentor: dr. sc. Marina Cindri, izv. prof. Povjerenstvo za ocjenu rada: dr. sc. Vianja Vrdoljak, doc. PMF dr. sc. Davor Kova evi, doc. PMF dr. sc. Nives Gali, doc.PMF Zamjena: dr. sc. Marina Cindri, izv. prof, PMF Rad prihvaen: __________________ BASIC DOCUMENTATION CARD University of Zagreb Diploma Thesis Faculty of Science Department of chemistry PREPARATION AND IDENTIFICATION OF POLYOXOMOLYBDATES VESNA CMRE KI Laboratory of General and Inorganic Chemistry, Faculty of Science, University of Zagreb, Ulica kralja Zvonimira 8, 10 000 Zagreb, Croatia ABSTRACT In this diploma thesis reactions of dichlorodioxomolybdenum(VI) (MoO2Cl2) with D,L- methionine, D,L- alanine, L-leucine and L-valine by addition of methanolic solution of morpholine or triethylamine or -picoline were investigated. All reactions were preformed in methanol: a) at room temperature, b) under reflux. Because of photosensitivity of the reactants and products the reactions were carried out in dark, and the chemicals were stored in dark place. Products were characterized by infrared spectroscopy, thermogravimetric analysis, X-ray diffraction on polycrystalline sample, electron paramagnetic resonance after exposure to UV-radiation and chemical analysis. Products were identified as polyoxomethoxomolybdates(VI) in which instead of amino acid binding, methoxo (-OCH3) group acted as a ligand to octamolybdate core. This can be explained by instability and sensibility of this class of compounds. It was concluded that the structure and molecular composition depend upon the reaction conditions. Following products were isolated and characterized: [C4H10NO]6[Mo8O26(OCH3)2], [C4H10NO]4[Mo8O26]2H2O, [C4H10NO]4[Mo8O24(OCH3)4], [C6H8N]4[Mo8O24(OCH3)4], [C6H8N]4[Mo8O24(OCH3)4]3CH3OH, triethylamonium octamolybdate and [Et3NH]2[MoO4]. The manuscript comprises: 61 pages, 29 pictures, 38 references, 4 tables. The original is written in Croatian language and deposited with Library of the Laboratory of General and Inorganic Chemistry, Faculty of Science, University of Zagreb. Key words: molybdenum(VI), octamolybdate, polyoxometalates, aminoacids, polyoxoalkoxomolybdates. Supervisor: dr. sc. Marina Cindri, associate professor Reviewers: dr. sc. Vianja Vrdoljak, assistant professor, PMF dr. sc. Davor Kova evi, assistant professor, PMF dr. sc. Nives Gali, assistant professor, PMF Substitute: dr. sc. Marina Cindri, associate professor, PMF Thesis accepted: _____________________________. 1.Uvod   Slika I: Molibdenit, ruda molibdena pribli~nog sastava MoS2. Diplomski rad Uvod ___________________________________________________________________________ 1.1. Svrha rada U ovom diplomskom radu ispitivane su reakcije diklorodioksomolibdena(VI) s aminokiselinama u metanolu, uz dodatak razli itih organskih baza. O ekivalo se da e reakcijom nastati polioksomolibdati s organskim ligandima (aminokiselinom ili alkoholom). Kompleksi polioksomolibdata s aminokiselinama zna ajni su za prou avanje interakcija izmeu organskih supstrata i kataliti ki aktivne povraine metalnog oksida te foto-oksidacijskih reakcija organskih spojeva. Do danas su sintetizirana dva kompleksa polioksomolibdata s aminokiselinama metioninom1 i lizinom2 te je rijeaena njihova struktura. Kemija polioksomolibdata u vodenim otopinama je dobro istra~ena dok je u drugim medijima slabije istra~ena. Zato se pokuaalo pripraviti komplekse polioksomolibdata u metanolu s: a) D,L-metioninom b) D,L-alaninom c) L-leucinom d) L-valinom. Diplomski rad Uvod ___________________________________________________________________________ Povijesni pregled  G odine 1778. slavni avedski flogistoni ar C. W. Scheele (slika 1) pripremio je iz minerala molibdenita (MoS2) oksid novog elementa i time prvi razlikovao mineral molibdenit od grafita.3 Nekoliko godina kasnije P. J. Hjelm izolirao je metal zagrijavajui mineral (MoO3) s ugljenom.3 Metal je dobio ime prema gr koj rije i molubdo( (molibdos) ato zna i olovo. Naime, molibdenit prije ovih otkria nisu razlikovali od ruda olova i grafita. Bioloaka va~nost molibdena je velika jer je sastavni dio kofaktora u viae od trideset enzima.4 Kofaktor je neproteinski dio enzima te esto ima ulogu aktivnog mjesta u enzimu. Meu najpoznatijim enzimima, koji sadr~e molibden u aktivnom mjestu, su nitrogenaza i enzimi iz skupine molibdopterina. Nitrogenaza se ubraja u skupinu hidrolaza, a izolirana je iz bakterija i modro-zelenih algi. Za enzime sulfit-oksidaze, ksantin-oksidaze i DMSO-reduktaze karakteristi no je da sadr~e molibdopterin (derivat dihidropterina).4 Molibden je u tim enzimima prisutan kao Mo(IV), Mo(V) i Mo(VI), a ligandi molibdena u enzimima su oksidi, sulfiti, tiolati, hidroksidi i neke aminokiseline. Najva~nija bioloaka funkcija molibdenskih enzima je kataliti ka reakcija prijenosa kisika s molibdena na supstrat uz sudjelovanje jednoelektronskih prijenosnih centara (Fe/S centri, citokromi, flavini). Molibden je u ljudskom tijelu zastupljen s manje od jedan posto masenog udjela.  K emija polioksometalata zapo ela je 1826. godine kada je `veanin Jns Jacob Berzelius (slika 2) pripravio [NH4]3[PMo12O40]. To je otvorilo potpuno novo podru je anorganske kemije. Ve 1862. godine Jean-Charles Galissard de Marignac uo ava dva strukturna izomera [SiW12O40]4- ime je zapo ela i strukturna karakterizacija polioksometalata. Ubrzo je slijedila prava eksplozija novih spojeva. Tako je ve 1908. godine zabilje~eno i analizirano viae od 750 polioksometalata.5 Diplomski rad Uvod ___________________________________________________________________________ Godine 1933. J. F. Keggin rjeaava kristalnu strukturu kubi nog H3[PW12O40]5H2O. Unapreivanje metoda, tehnika i teorija koje su objasnile koordinacijsku kemiju (1893. Alfred Werner  Teorija koordinacije) krajem 19. i ranih godina dvadesetog stoljea pridonijelo je sve veem znanju i interesu za kemiju polioksometalata.6 Danas polioksometalati ine nesagledivu klasu polinuklearnih okso-anionskih klustera prijelaznih metala kao ato su molibden (Mo), volfram (W), vanadij (V) ili kombinacije tih metala. Godine 1996. zabilje~eno je ak 700 publikacija i patenata polioksometalata.7 Primjena polioksometalata posljedica je njihovih izuzetnih redoks i kiselinsko-baznih svojstava, termi ke stabilnosti i strukturne raznolikosti. Polioksometalati zanimljivi su i kao materijali zbog veli ine aupljina u strukturi U analiti koj kemiji koriste se za dokazivanje i odreivanje preko 26 elemenata.8 Veina danaanjih istra~ivanja usmjerava se na supramolekularna svojstva, kataliti ka svojstva polioksometalata te njihovu moguu primjenu u lije enju tumora9, virusnih10 i retrovirusnih10 bolesti. 2.Literaturni pregled   Slika II: Vulfenit, ruda molibdena pribli~nog sastava PbMoO4. Diplomski rad Literaturni pregled ___________________________________________________________________________ 2.1. Strukturna svojstva polioksometalata Polioksometalate susreemo u kemiji vanadija, niobija, tantala, volframa i molibdena u visokim oksidacijskim stanjima. To su diskretne molekule nanometarske veli ine, koje sadr~e viae od 4 metalna centra, nastale povezivanjem MOn poliedara gdje je n koordinacijski broj metala. Koordinacijski broj uglavnom je n = 6 (slika 3) (oktaedarska koordinacija), ali mo~e biti i n = 4, 5, ili 7.  Slika  SEQ Slika \* ARABIC 3: Prikaz strukturne jedinice polioksometalata. MO6 je deformirani oktaedar C4v simetrije.5 Osim kisikovih atoma na metalni centar mogu biti vezani heteroatomi koji se ozna avaju simbolom X. Viae od 60 elemenata, uklju ujui veinu nemetala i prijelaznih elemenata mo~e imati funkciju heteroatoma. Ovisno o prisustvu heteroatoma, polioksometalati se dijele na izopolianione i heteropolianione: izopolioanion (IPA)  [MmOy]p- heteropolianion (HPA)  [XxMmOy]q-, x d" m. Heteropolianioni koji sadr~e viae razli itih metalnih atoma nazivaju se mijeaani - addenda klusteri. Povezivanjem osnovnog strukturnog motiva, oktaedra MO6 (ponekad i MO5) preko bridova, vrhova ili stranica (slika 4) nastaju klusterske strukture polioksometalata. Najpovoljnije povezivanje dvaju oktaedra odreeno je odbijanjima izmeu metalnih centara koje je najmanje pri vezivanju oktaedara preko vrhova ili bridova dok je povezivanje preko stranica termodinami ki nepovoljno.6 Udaljenosti izmeu metalnih centara u nekim polioksometalatima prikazane su u Tablici 1. Diplomski rad Literaturni pregled ___________________________________________________________________________  Slika  SEQ Slika \* ARABIC 4: Poliedarski modeli prikazuju mogue na ine povezivanja MO6 strukturnih jedinica: a) preko vrhova, b) preko bridova i c) preko stranica. Tablica  SEQ Tablica \* ARABIC 1: Udaljenosti M  M u strukturama s razli itim na inom vezivanja MO6 oktaedara.6 MetalOktaedri povezani preko vrhova / Oktaedri povezani preko bridova / W(VI)3,73,4Mo(VI)3,53,5V(V)3,53,2 Omjer naboj/polumjer metalnog iona, odnosno koordinacijski broj te  - akceptorska svojstva metala odreuju fizikalno  kemijska svojstva i stabilnost polioksometalata. Stabilnosti polioksometalata pridonosi stvaranje dvostruke veze p-d interakcijom metala s terminalnim kisikovim atomima.11 Upravo zato samo metali odreenog omjera naboj/polumjer i oni s praznim d-orbitalama stvaraju polioksometalate. Sinergi no djelovanje dvostruke veze s terminalnim kisikovim atomima te jaka polarizirljivost kisika, uzrokuju deformaciju oktaedra u smislu pomaka centralnog metalnog atoma prema terminalnom kisikovom atomu. Jaka polarizacija M=O veze uzrok je velike kiselosti (pKa ~ 0-2) jer je pozitivni dio dipola orijentiran prema vanjskoj strani polioksometalata i sprje ava vezanje protona na kisik.11 Time je takoer kontroliran i stupanj polimerizacije i zato nikada ne nastaju polimerne mre~e ili lanci, ve diskretne molekule polioksometalata.11 Diplomski rad Literaturni pregled ___________________________________________________________________________ Povezivanjem poliedara stvaraju se upljine pa se strukture polioksometalata mogu ponekad promatrati kao klatrati u kojima razlikujemo vanjski i unutarnji (eng. incapsulated) dio. Takve strukture su Kegginova tipa (slika 5), Lindqvist struktura (slika 8) i Wells Dawsonova struktura (slika 7) koje se mogu prikazati opim formulama U%V u kojima U ozna ava unutarnji dio, a V vanjski dio:6 Kegginov tip strukture  [XO4]n- % M12O36 Wells  Dawsonova struktura- [XO4]2n- % M18O54 Lindqvist struktura  O2- % M6O18.  Slika  SEQ Slika \* ARABIC 5: Prikaz strukture Kegginova tipa.   Slika  SEQ Slika \* ARABIC 6: Prikaz Anderson Evans strukture. Slika  SEQ Slika \* ARABIC 7: Prikaz Wells Dawson strukture. Diplomski rad Literaturni pregled ___________________________________________________________________________ Veina heteropolianiona ima Wells  Dawsonovu strukturu ili strukturu Kegginova tipa, dok izopolianioni imaju esto Anderson  Evans strukturu (slika 6) ili Lindqvist strukturu  M6O19n- (slika 8).  Slika  SEQ Slika \* ARABIC 8: Prikaz Lindqvist strukture. Postoje razli iti izomerni oblici strukture Kegginova tipa (slika 9), a njihovo nastajanje ovisno je o pH otopine. -izomer strukture Kegginova tipa, simetrije Td graen je od 12 istih MO6 oktaedara spojenih preko bridova ili vrhova s centralnim XO4 tetraedrom. U strukturi se razlikuju tri vrste veza metal  kisik: dvostruka M=O veza (terminalni kisik), jednostruka M-O veza (kisik u srediatu tetraedra) i premoaujua M-O-M veza (premoaujui kisik). - i - izomeri strukture Kegginova tipa, C3v simetrije, graeni su od etiri M3O13 strukturne jedinice spojene preko bridova, a nastaju rotacijom jedne, odnosno dvije jedinice za 60 oko osi treeg reda -izomera.6  Slika  SEQ Slika \* ARABIC 9: Poliedarski prikaz strukturnih izomera strukture Kegginova tipa i njihova simetrija. Zatamnjeni oktaedri povezani su preko bridova.6 Diplomski rad Literaturni pregled ___________________________________________________________________________ 2.2. Fizikalno - kemijska svojstva polioksometalata Kvalitativno prou avanje molekulskog elektrostatskog potencijala strukture polioksometalata od velikog je zna aja za odreivanje nukleofilnih regija u strukturi.6 Elektrostatski potencijal prikazuje se 3D-plohom ija boja je funkcija molekulskog elektrostatskog potencijala. Crvena podru ja prikazuju nukleofilne regije, a plava elektrofilne regije. Na slici 10 prikazan je molekulski elektrostatski potencijal za SiMo3W9 i SiV3W9 derivate. Iz tog prikaza jasno se vidi utjecaj omjera naboj/polumjer metala na polarizaciju metal  kisik veze te se potvruje kiselost polioksometalata. Takoer se primjeuje da su premoaujui kisikovi atomi bazi niji (nukleofilniji) od terminalnih kisikovih atoma. Uo ava se i jaka bazi nost u unutraanjosti strukture koja potje e od kisika smjeatenog u centru tetraedra metalnih iona ato ih ini iznimno nedostupnim protonima iz otopine.  Slika  SEQ Slika \* ARABIC 10: Poliedarski prikaz i 3D-ploha molekulskog elektrostatskog potencijala derivata SiMo3W9 i SiV3W9, iz razli itih perspektiva.6 Diplomski rad Literaturni pregled ___________________________________________________________________________ Svaki metalni ion koji ima jedan terminalni kisikov atom ima praznu dxy  orbitalu u koju mo~e primiti elektrone. Zbog toga su polioksometalati, u kojima svaki metalni centar ima jedan terminalni kisikov atom (C4v simetrija), jaka oksidacijska sredstva. Ubrajaju se u aninone Tipa I, a imaju strukture Kegginova tipa, Wells  Dawsonovu i Lindqvistovu strukturu.12 Njihovom redukcijom nastaju karakteristi no plavi poliokosometalati (heteropoly blues) slo~enih struktura koji su klasificirani kao spojevi  mijeaanih valencija jer ne dolazi do redukcije svih metalnih centara. Nastalim redukcijskim produktima struktura nije bitno razli ita od ishodnog spoja12 budui da elektroni popunjavaju neveznu orbitalu te su delokalizirani kroz nekoliko atoma. Postoje dva mehanizma delokalizacije elektrona: a)5 termi ki pobueno preskakanje elektrona izmeu metalnih centara i b)5 delokalizacija u osnovnom stanju koja se ostvaruje -vezivanjem reduciranih metalnih atoma sa susjednim atomima preko premoaujuih kisikovih atoma. Daljnjom redukcijom nastaju smei produkti (heteropoly brownes) u kojima nema delokalizacije elektrona u strukturi. Polianioni Tipa II (npr. Andersonove strukture) imaju metalni atom koordiniran s dva (cis) terminalna kisikova atoma.12 Takav metalni atom nema praznih d-orbitala i ne podlije~e redukciji. Redukcijska svojstva polioksometalata i nastanak plavih produkata nalaze primjenu u analiti koj kemiji za kvantitativna odreivanja udjela nekog elementa u analitu. Na primjer, redukcijom otopine molibdata (MoO42-) ili MoO3 nekim redukcijskim sredstvom kao ato su hidrazin, sumporov dioksid ili Sn2+ ioni dolazi do pojave plave boje. To svojstvo koristi se za spektrofotometrijsko odreivanje fosfatnih i arsenatnih iona, kositra kao i samih redukcijskih sredstava.13 Polioksometalati su izolirani iz vodenih i nevodenih otopina pri kiselim uvjetima (shema 1). Nastaju polimerizacijom iona MO42 tetraedarske simetrije, a ovisno o pH nastaju razli ite klusterske strukture.  7MoO42- + 8H+ [Mo7O24]6- + 4H2O (1) 12WO42- + HPO42- + 23H+ [PW12O40]3- + 12H2O Kristalizacija se poti e dodatkom iona suprotnog naboja (H+, protonirana organska baza, kationi alkalijskih metala i sl.). Diplomski rad Literaturni pregled ___________________________________________________________________________ Topljivost soli polioksometalata ovisi o relativnim odnosima izmeu energije kristalne reaetke, energije solvatacije i interakcijama meu molekulama otapala. Za tipi ne heteropolianione energija kristalne reaetke i energija solvatacije prili no su niske6 pa je veina polioksometalata dobro ili umjereno topljiva u vodi, osim soli velikih organskih kationa koje su topljive u nepolarnim organskim otapalima.11 2.3. Polioksometalati molibdena(VI) Polioksometalati molibdena(VI) nastaju polimerizacijom tetraedarskog molibdatnog iona MoO42 (slika 11) sni~avanjem pH vrijednosti otopine ispod pH = 6 (shema 2). Pri tome sukcesivno nastaju anioni heptamolibdat [Mo7O24]6-, a zatim oktamolibdat [Mo8O26]4- i kluster [Mo36O112(H2O)16]8-.12 Pri vrlo kiselim uvjetima (ispod pH = 2) iz otopine molibdata talo~i ~uti hidratizirani molibdenov trioksid, MoO32H2O.  7MoO42- + 8H+ [Mo7O24]6- + 4H2O (2) [Mo7O24]6- + MoO42- + 4H+ [Mo8O26]4- + 2H2O.  Slika  SEQ Slika \* ARABIC 11: Struktura tetraedarskog molibdata [MoO4]2-.14 Meuprodukti reakcije (2) su mogui te se mogu izolirati podeaavanjem pH i koncentracije otopine, temperature i brzinom kristalizacije. Naj eae kristaliziraju smjese razli itih aniona i polianiona: dimolibdat [Mo2O7]2-, heksamolibdat [Mo6O19]2- i dekamolibdat [Mo10O34]8-. Ovisno o prisutnom kationu, nastaju polimerne strukture [Mo2O7]2- aniona graene od beskona nih lanaca MoO6 oktaedara i MoO4 tetraedara ili diskretne molekule. Rentgenskom strukturnom analizom utvreno je da je [NH4]2[Mo2O7] polimerne strukture.15 Isto tako utvreno je da [Bu4NH]2[Mo2O7], izoliran iz otopine acetonitrila dimerna molekula.16 Diplomski rad Literaturni pregled ___________________________________________________________________________ Sintetizirano je nekoliko soli [Mo6O19]2- aniona (slika 12) te im je odreena kristalna struktura rentgenskom strukturnom analizom. Polianion je izostrukturan s [Nb6O19]8- i ne pokazuje zna ajno odstupanje od Oh simetrije.12 Ubraja se u Tip I polianiona, Lindqvistove strukture te se mo~e reducirati do  mijeaanih [Mo6O19]3- i [Mo6O19]4- polianiona.12 Oksidirani polianioni ~ute su boje (max = 325 nm) za razliku od ostalih izopolimolibdata koji su bezbojni. Hidrotermalnom sintezom uz reducens hidroksilamin hidroklorid sintetizirana je prva molibdenska bronca [NH4][Mo6O18] s prosje nom valencijom molibdenovih atoma 5,83, te joj je odreena heksagonska struktura.18 Heptamolibdat (paramolibdat) u protoniranom obliku [HnMo7O24](6-n)-, n = 1-3, postoji u vodenim otopinama pri pH ~ 3-5.12 Rentgenskom strukturnom analizom odreene su strukture amonijeve, natrijeve, kalijeve i izopropilamonijeve soli heptamolibdata s cis-MoO2 stereokemijom svakog metalnog atoma (slika 13). Heptamolibdat pripada polianionima Tipa II pa ne posjeduje oksidacijska svojstva. Ovaj izopolianion ima D3d simetriju.12  Slika  SEQ Slika \* ARABIC 13: Trodimenzijska kristalna struktura heptamolibdtata, crveno  kisik, zeleno  molibden.19(CSD) Utjecaj kationa na strukturu izoliranog spoja uo ava se na primjeru dimolibdata koji je stabilan u acetonitrilnim-vodenim otopinama, ali dodatkom kationa alkalijskog metala dolazi do kristalizacije soli heptamolibdata. Diplomski rad Literaturni pregled ___________________________________________________________________________  Oktamolibdat(VI) egzistira u vodenim i nevodenim medijima u obliku tri mogua izomera: -[Mo8O26]4- 20, -[Mo8O26]4- 21 i -[Mo8O26]4- 1 izomer koji je meuprodukt reakcije izomerizacije !. Izomeri - i - izolirani su iz kiselih otopina (pH = 3-4) kao alkilamonijeve, alkilpridinijeve, alikilfosfonijeve, anilinijeve ili t-butil-amonijeve soli. Izomer -[Mo8O26]4" graen je od aest {MoO6} oktaedara povezanih preko bridova koji se nalaze iznad i ispod {MoO4} tetraedra. Izomer -[Mo8O26]4" (slika 14) graen je od osam {MoO6} oktaedara povezanih preko bridova, dok -[Mo8O26]4" izomer sadr~i aest {MoO6} oktaedara povezanih preko bridova i dvije {MoO5} trigonske bipiramide povezane preko dva brida s oktaedrima. Veliki afinitet prema slobodnom koordinacijskom mjestu u {MoO5} trigonskoj bipiramidi pokazuju O-donorski ligandi ijim vezanjem dolazi do koordinacijskog zasienja i promjene koordinacije iz trigonsko bipiramidalne u oktaedarsku. Zabilje~eni su takoer - i - izomeri oktamolibdata. Izomer -[Mo8O26]4" ima prijelaznu strukturu u reakciji izomerizacije ! ili !, a -[Mo8O26]4" izomer sadr~i aest {MoO5} kvadratnih piramida i dva {MoO6} oktaedra.22 Vezanjem organskih, prete~no N- ili O-donorskih liganada na oktamolibdatnu jezgru nastaju derivati -[Mo8O26]4" sa zasienom oktaedarskom koordinacijom, ope formule [Mo8O26Lm](2n+4) (m = 2, 4) gdje je n nabojni broj liganda L koji se ve~e (slika 15).  (B) Slika  SEQ Slika \* ARABIC 15: Poliedarski prikaz na ina vezivanja liganada na oktamolibdatnu jezgru.1 Diplomski rad Literaturni pregled ___________________________________________________________________________ Izolirani su derivati [NH4]6[Mo8O26(O2CH)2]2H2O, Na2[Mo8O26(L-LysH2)2]8H2O (lysH2 = lizin) i [HMorph]4[H2Mo8O26(Met)2]4H2O (Morph = morfolin, Met = metioninato) s O-donorskim ligandima, [Hpy]4[Mo8O26(py)2]2Me2SO (py = piridin) i K6[Mo8O26(NCS)2]6H2O s N-donorskim ligandima koji imaju strukturu tipa A prikazanoj na slici 15.1 Derivati H4[Mo8O24(Met)4]4H2O, H4[Mo8O24(Met)4]8MeOH (MeOH = metanol) i Na4[Mo8O24(OMe)4]8MeOH (OMe = metokso) imaju strukturu tipa B prikazanoj na slici 15.1 Ligandi L i L' u strukturi tipa B meusobno su u cis-polo~aju, s time da su L terminalno vezani ligandi, a L' su premoaujui ligandi. 2.3.1. Derivati polioksomolibdata(VI) s aminokiselinama U otopini kod fizioloakog pH aminokiseline postoje u obliku zwiteriona  amino skupina je protonirana, a karboksilna disocirana. U kiselim otopinama, aminokiseline su pozitivno nabijene, a u lu~natima negativno. Karboksilna i amino skupina, a ponekad i bo ni ogranak ako sadr~i heteroatom, mogu djelovati kao ligandi prema metalnom ionu. Monodentatnu koordinaciju aminokiselina preko atoma duaika amino skupine nalazimo u otopinama kineti ki inertnih metalnih iona poput kroma(III), kobalta(III), iridija(III), platine(II) i rodija(II), dok monodentatna koordinacija preko slabijeg O-donorskog atoma karboksilne skupine nije esta, ali je nalazimo kod kobalta(III), platine(II) i molibdena(VI).23 Do monodentatnog vezanja aminokiselina na metal dolazi pri pH = 3-5 ili kada su ili N- ili O- donorski atomi blokirani supstitucijom. Uobi ajeni na in koordinacije aminokiselina na metal je didentatno kelatiranje preko N- i O- donorskog atoma pri emu nastaje termodinami ki stabilan petero lani prsten. Konstante nastajanja kompleksa uvelike ovise o pH otopine, odnosno koncentraciji odreenog ioniziranog oblika aminokiseline. Aminokiseline koje u bo nom ogranku sadr~e heteroatom, potencijalni su tridentatni ligandi. Oktamolibdat preferira O-donorske ligande pa se aminokiseline koordiniraju monodentatno preko kisika karboksilne skupine pri emu iz potpuno simetri nog nastaje kiralan, opti ki aktivan derivat polioksomolibdata. Diplomski rad Literaturni pregled ___________________________________________________________________________ Iz metanolne otopine diklorodioksomolibdena(VI) (MoO2Cl2) uz aminokiselinu metionin i morfolin, nakon prekristalizacije iz vode izolirana je sol [HMorph]4[Mo8O24(OH)2(Met)2]4H2O (slika 16).1 Rentgenskom strukturnom analizom utvreno je osam centrosimetri nih oktaedara povezanih preko bridova (koordinacijski zasien derivat -oktamolibdata), produljenje veza Mo-O zbog trans utjecaja terminalnih kisikovih atoma i vezanje metionina preko kisika karboksilne skupine jednostrukom Mo-O vezom na Mo(VI). Iz vodene otopine diklorodioksomolibdena(VI) i metionina izoliran je derivat [Mo8O20(OH)4(Met)4]4H2O kao bijeli talog, a iz metanolne otopine pri povienoj temperaturi izoliran je metanolni solvat [Mo8O20(OH)4(Met)4]8MeOH.1 Iz tih primjera vidljiv je utjecaj otapala i eksperimentalnih uvjeta na sastav izoliranog spoja.  Slika  SEQ Slika \* ARABIC 16: Trodimenzijski prikaz strukture [HMorph]4[Mo8O24(OH)2(Met)2]4H2O.1 (CSD) Heteromolibdatima Kegginova tipa i heteromolibdatima s heptamolibdatom kao fragmentom ispitivana je antitumorska9,24 i antiviralana10,24 aktivnost. Utvreno je da se heptamolibdat ve~e u omjeru 1:1 s FMN  kompleksom u mitohondriju tumorske stanice te inhibira stvaranje ATP-a, izvora ~ivotne energije stanice.2 Posljedica je odumiranje tumorske stanice. Diplomski rad Literaturni pregled ___________________________________________________________________________ Istra~ivanja strukturne kemije polioksomolibdata s organskim ligandima pru~aju uvid u njihovo antitumorsko i antiviralno djelovanje, slu~e kao modeli kataliti kih mjesta u molibdoenzimima8 i za bolje razumijevanje interakcija izmeu organskog supstrata i kataliti ki aktivne povraine metalnih oksida.25 S tim ciljem sintetiziran je derivat -oktamolibdata, Na2[Mo8O26(L-lysH2)2]8H2O iz vodene otopine molibdata (pH = 3) te mu je odreena kristalna struktura rentgenskom strukturnom analizom.2 Utvreno je vezanje lysH2 s molibdenom preko kisika karboksilne skupine jednostrukom vezom te intermolekularne vodikove veze izmeu protoniranih amino skupina lizina te kisika oktamolibdata duljine 2,7  2,9 (slika 17).2  Slika  SEQ Slika \* ARABIC 17: Prikaz Na2[Mo8O26(L-lysH2)2]8H2O strukture s vidljivim intermolekularnim vodikovim vezama izmeu duaika protoniranih amino skupina lizina te kisika oktamolibdata (obraeno Mercury programom). Diplomski rad Literaturni pregled ___________________________________________________________________________ 2.3.2. Polioksoalkoksomolibdati(VI) Od prvih istra~ivanja u svjetskom istra~iva kom centru du Point 1980.-tih, polioksoalkoksometalati ine najveu i naj eae istra~ivanu skupinu derivata polioksometalata. Uzrok tome je laka priprava ove vrste spojeva. Mogui putevi sinteze su22: O-alkilacija polioksometalata s trialkiloksonijevim solima, dialkilsulfatima ili halogenalkanima, termoliza trialkiloksonijevih i arildiazonijevih soli, esterifikacija polioksometalata s alkoholom, kontrolirana hidroliza metalnih alkoksida, reakcija oksida s alkoholima, samoudru~enjem polioksometalata i alkohola. Derivati polioksomolibdata(VI) s metanolom dobri su modeli metalnih oksida - katalizatora reakcije oksidacije metanola u formaldehid. Godine 1983. refluksiranjem MoO32H2O u suviaku metanola sintetiziran je Na4[Mo8O24(OMe)4]"8MeOH (slika 18) ijom pirolizom nastaje formaldehid, CH2O i voda.26 Na temelju njegove strukture pretpostavljen je mehanizam oksidacije metanola u formaldehid.  Slika  SEQ Slika \* ARABIC 18: Struktura Na4[Mo8O24(OMe)4]"8MeOH, zeleno  molibden, crveno  kisik, ljubi asto-natrij, sivo  ugljik, bijelo  vodik (CSD).26 Diplomski rad Literaturni pregled ___________________________________________________________________________ Metodom rentgenske strukturne analize utvreno je postojanje dvaju [Mo8O24(OMe)4]4- aniona i dvaju kristalografski nezavisna [Na2(CH3OH)4]2+ kationa (slika 18).26 Najsporiji korak reakcije oksidacije metanola u formaldehid je kidanje C-H veze u metokso skupini i prijenos protona s metokso skupine na susjedne kisikove atome. Kao model metokso-MoO3 meuprodukta ove reakcije, zanimljive su konformacije metokso grupa u [Mo8O24(OMe)4]4- anionu. Utvrena su tri kratka (ispod 2,5 duljine) C%HO intramolekulska kontakta u [Mo8O24(OMe)4]4- anionu te usmjerenje metokso skupine tako da je omoguen prijenos samo jednog protona na akceptorske atome kisika (Mo=O) ato je dokaz pretpostavljenog mehanizma katalizirane reakcije oksidacije.26 Sintetizirani su i derivati tetranuklearnih heteropolimolibdata s alkoholima analognih svojstava. 2.3.3. Fotokromizam polioksomolibdata(VI) Fotoosjetljiv materijal definira se kao onaj ija se apsorpcijska svojstava (boja) mijenjaju prilikom opti kog pobuivanja, a ija se obojenost nakon uklanjanja izvora zra enja zadr~ava. Ta pojava promjene boje zove se fotokromizam. Kod polioksometalata fotokromizam je primijeen prije otprilike devedeset godina na -Kegginovom volframatu H3[PW12O40]. Njegovom fotokemijskom redukcijom (UV, g-zra enje) nastaje plavi produkt (hetropoly blue), koji se oksidira djelovanjem kisika ili drugih oksidansa kao ato je Fe3+, AgNO3 i H2O2.27 Elektronski spektri polioksometalata, u kojima se metali nalaze u najviaim oksidacijskim stanjima (d0), posljedica su prijelaza elektrona s liganda na metal (LMCT  ligand-to-metal-charge transfer), odnosno s kisika na metal pri emu nastaje kompleks prijenosa naboja. LMCT prijelazi karakteristi ni su samo za kompleksne spojeve i ne nalaze se u spektru slobodnog liganda ili slobodnog metalnog iona.28 Mehanizam prijenosa uklju uje prijelaz elektrona iz 2p-orbitala kisika u energetski viaa stanja, veinom d-orbitale metala (shema 3) pri emu dolazi do redukcije metalnog centra. Pritom mogui prisutni heteroatom ili pozitivna  rupa (kation, ne istoe, defekti) u strukturi djeluju kao  stupice za elektrone, tj. lokalizirani energetski nivoi u O!M LMCT prijelazu.27 Da bi se elektron  oslobodio iz  stupice mora savladati energetsku barijeru E za ato je potrebno termi ko ili opti ko pobuivanje. Diplomski rad Literaturni pregled ___________________________________________________________________________  Shema 3: Prikaz prijenosa elektrona u polioksometalatima: a)stvaranje nosioca naboja, b) elektronska stupica, c) otputanje elektrona stimulacijom, d) rekombinacija elektrona i pozitivnih rupa.27 Relaksacija O!M LMCT prijelaza je neradijativni proces, kod kojeg dolazi do rekombinacije pozitivnih  rupa i elektrona unutar energijske  aupljine , te radijativni proces intramolekulskog prijenosa energije koji odgovara O!M LMCT energijskoj  aupljini . Uz LMCT prijelaze mogui su i d-d prijelazi d1 elektrona izmeu t2g i eg orbitala metalnog iona u vidljivom dijelu spektra, ali u usporedbi s LMCT prijelazima esto su zanemarivo mali.28 U literaturi fotokromizam je dobro objaanjen na alkilamonijevim polioksomolibdatima(VI), fotoosjetljivim u krutom stanju i u otopini. Pobuivanjem O!Mo LMCT prijelaza UV zra enjem ( < 400 nm) nastaje metastabilni kompleks prijenosa naboja MoVO5(OH) (shema 4).27 Pri nastanku kompleksa dolazi do prijenosa vodika s duaika alkilamonijevog kationa na premoaujui kisikov atom u {MoO6} poliedru te interakcije  pozitivnog kisikovog atoma nastalog O!Mo prijelazom s neveznim elektronima duaikovog atoma amino skupine. Metastabilno stanje MoVO5(OH) dokazuje se metodom elektronske paramagnetske rezonancije (EPR) ili magnetokemijskim mjerenjima.  Shema 4: Mehanizam nastanka kompleksa prijenosa naboja MoVO5(OH).27 Diplomski rad Literaturni pregled ___________________________________________________________________________ Ovisno o stupnju redukcije, o broju fotoreduciblinih {MoO6} mjesta u kristalnoj reetci i delokalizaciji d1 elektrona na metalnom centru, koja ovisi o M-O-M kutu, odnosno d-p-d orbitalnom preklapanju, ozra eni uzorak je tamnoplave ili smee boje.27 Broj fotoreducibilnih mjesta odreuje se posebnom tehnikom snimanja i analize EPR spektra monokristala.27 Reverzibilna reakcija mogua je kod polianiona Tipa I u atmosferi kisika i u mraku. Promjena boje iz bijele u smeu zapa~ena je kod mnogih anilinijevih i piridinijevih soli -oktamolibdata: [NH3C6H5]4[Mo8O26]2H2O, [NHMe2C6H5]4[Mo8O26]2H2O.27 Kod polioksomolibdata koordiniranih s organskim ligandom poput aminokiseline ili alkohola takoer je opa~en fotokromizam: Na4[Mo8O24(OMe)4]8H2O (bijelo ! plavo), [HMorph]4[Mo8O24(Met)2]4H2O, Na2[Mo8O26(L-H2Lys)2]8H2O (Morph = morfolin, Met = metioninato, Lys = lizin) (bijelo ! smee).27 2.3.4. Velike klusterske strukture s polioksomolibdatnim jezgrama Povezivanjem osnovnih fragmenata: {Mo1}, {Mo2}, {Mo(Mo)5}, {Mo8}, ({Mo8}{Mo1}) i {Mo11} (slika 19) meusobno ili preko drugih koordinacijskih centara nastaju klusterske strukture polioksomolibdata. {Mo(Mo)5} strukturna jedinica sastoji se od MoO6(OH2) pentangonske bipiramide povezane preko bridova s pet MoO6 oktaedara.29 Ovakva strukturna jedinca nalazi se u sferi nim kepleratima  nanometarskim, klusterima polioksomolibdata ikozaedarske simetrije. Prvi takav, visokosimetri ni superfuleren {Mo132}, sintetizirao je Achim Mller 1998. godine (slika 20) te mu je dao naziv keplerat jer dijelovi strukture podsjeaju na rani svemir Johannesa Keplera.13 {Mo(Mo)5} strukturna jedinica nalazi se i u {Mo72Fe30} klusteru (slika 21), takoer je ikozaedarske simetrije.30 {Mo(Mo)5} strukturne jedinice povezane su meusobno {Mo2} fragmentima (oktaedri spojeni du~ stranica). Diplomski rad Literaturni pregled ___________________________________________________________________________  {Mo1} {Mo2} {Mo(Mo)5} {Mo8}  {(Mo8)(Mo1)}  {Mo11} {Mo11} Slika  SEQ Slika \* ARABIC 19: Poliedarski prikaz strukturnih jedinica polikosomolibdata.31  Slika  SEQ Slika \* ARABIC 20: Kluster {Mo132}, sadr~i 12 {Mo(Mo)5} strukturnih jedinica (svjetloplavo) i 30 MoO6 oktaedara (crveno). Diplomski rad Literaturni pregled ___________________________________________________________________________  Slika  SEQ Slika \* ARABIC 21: Struktura {Mo72Fe30} klustera (lijevo; Mo: plavo, Fe: ~uto, O: crveno) i upisani Fe30 ikozododekaedar (desno).30 {Mo8} strukturna jedinica graena je od centralne {MoXO6} bipiramide povezane s pet {MoO6} oktaedara preko vrhova, od kojih su etiri povezana s druga dva {MoO6} oktaedara preko vrhova (slika 22a). Povezivanjem {Mo8} strukturnih jedinica preko {Mo1} fragmenata nastaju klusteri {Mo17}, {Mo36}, {Mo57} i {Mo154}. Kluster {Mo17} (slika 22b, c) nastaje iz dvije {Mo8} strukturne jedinice povezane preko osam kisikovih atoma i jednog atoma Mo.32  Slika  SEQ Slika \* ARABIC 22: Nastajanje klustera{Mo17}.32 Diplomski rad Literaturni pregled ___________________________________________________________________________ Kluster {Mo57} (slika 23) ima D3h simetriju, a graen je od tri {Mo17} fragmenata izmeu kojih se nalaze tri velike aupljine u koje se lako koordiniraju elektrofilni M-O fragmenti kao ato je {MoO}4+. To omoguuje rast klusterske strukture i nastanak {Mo57+xM6} (x = 0  6) struktura.   Slika  SEQ Slika \* ARABIC 23: Ball-and-stick prikaz {Mo57M6} strukture s naglaenom M6 trigonskom prizmom (Mo-plavo, O-crveno, Fe-zeleno) i poliedarski prikaz {Mo57M6} strukture s vidljivim upljinama na povrini strukture. Promjer unutranje upljine aniona {Mo57} koju ini {O33} poliedar je ~0,9 nm okomito na S3 os i 0,5 nm paralelno s S3 osi.16 `upljina je dostupna preko dvije  rupe koju ine planarni i alternirajui Mo-O-M-O 12-tero lani prstenovi u klusterskoj ljusci smjeatenih du~ S3 osi. Dijamagneti ni izopolianionski kluster airine 4 nm {Mo154} (slika 24) sintetiziran je ranih '90.-tih u laboratoriju prof. Mllera, a graen je od 154 molibdenovih atoma uklopljenih u slagalinu kisikovih atoma.13 Godine 1995. Mller objavljuje sintezu amonijeve soli [Mo154(NO)14O420(OH)28(H2O)70](255) tetradekamera pribli~no D7d simetrije, klustera graenog od 140 {MoO6} oktaedra i 14 {Mo(NO)O6} pentagonskih bipiramida sa sredianjom aupljinom promjera 20 .32 Svaka od 14 podjedinica je zapravo {Mo8} fragment koji sadr~i sredianju {Mo(NO)O6} pentagonsku bipiramidu vezanu sa 7 razli itih {MoO6} oktaedra preko vrhova i bridova. Diplomski rad Literaturni pregled ___________________________________________________________________________ Profesor Mller nije stao na razini {Mo154} klustera te je 1999. godine sintetizirao {Mo176} (heksadekamer) (slika 24a), a ubrzo i {Mo368} kluster (slika 24b) koji je intenzivno plave boje zbog delokalizacije elektrona, s dimenzijama proteinske molekule, sa svojstvima zeolita i moguom primjenom u selektivnoj katalizi i kao nanoreaktor.   A B Slika  SEQ Slika \* ARABIC 25: a) Poliedarski prikaz {Mo176} klustera i b) {Mo368} s unutranjom upljinom 2,5 nm irokom i 4,5 nm dugom u kojoj je zarobljeno 400 molekula vode. 3.Eksperimentalni dio  Slika III: Povelit, ruda molibdena pribli~nog sastava CaMoO4. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ Priprava diklorodioksomolibdena(VI), MoO2Cl2 Diklorodioksomolibden(VI), MoO2Cl2 koriten je kao polazni spoj u svim reakcijama sinteze te je s tom svrhom pripremljen. Uzorak 0,2 g aktivnog ugljena i 2 g molibdenovog trioksida, MoO3 pomijeano je u posudici za vaganje i sueno jedan sat na 100 C u suioniku. Smjesa aktivnog ugljena i molibdenovog trioksida u porculanskoj laici stavljena je u reakcijsku cijev aparature. Kroz aparaturu je propuatan klor nekoliko minuta da istisne zrak, a reakcijska cijev blago je zagrijavana da se istjera vlaga. Klor je razvijan dokapavanjem teh. konc. klorovodi ne kiseline, HCl(aq) na kalijev permanganat, KMnO4(s). Reakcija zapo inje grijanjem reakcijske cijevi u podru ju porculanske laice auateim plamenom ime nastaju ~uti kristalii diklorodioksomolibdena(VI), MoO2Cl2. Nastali produkt brzo se prebaci u zatamnjenu bocu i dobro za epi budui da se pod utjecajem svjetlosti i vlage lako reducira ato se vidi po pojavi plave boje. Reakcije diklorodioksomolibdena(VI) s aminokiselinama i morfolinom Namjera je bila sintetizirati derivat -[Mo8O26]4" koordiniran s aminokiselinama D,L- metioninom, D,L-alaninom, L-leucinom i L-valinom kao morfolinijeve soli, ope formule [HMorph](2n+4)[Mo8O26Lm](2n+4) (m = 2, 4) gdje je n naboj liganda L koji se ve~e. Reakcije su izvedene pri sobnoj i poviaenoj temperaturi u metanolu. 3.2.1. Reakcije diklorodioksomolibdena(VI) s D,L-metioninom, D,L-alaninom, L-leucinom, L-valinom i morfolinom pri sobnoj temperaturi Metanolnoj otopini (20 cm3) diklorodioksomolibdena(VI) (0,5 g, 2,51 mmol) i D,L- metionina (0,094 g, 0,628 mmol) dodana je 10 % otopina morfolina u metanolu do po etka talo~enja produkta. aaa zaatiena crnom folijom od svjetlosti zbog mogue fotoosjetljivosti spoja, ostavljena je stajati par dana radi potpunije kristalizacije. Bijeli, praakasti produkt (0,42 g,  = 75 %) otfiltriran je i dobro ispran metanolom. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ Na isti na in izolirani su bijeli, praakasti produkti prireivani s dodatkom aminokiselina D,L-alaninom, L-leucinom i L-valinom. Svim pripravljenim spojevima snimljen je IR spektar, rentgenogram praha te je kvantitativno odreen sadr~aj molibdena kemijskom i termogravimetrijskom analizom. Napravljen je i kvalitativan test na kloride. Budui da su IR spektar i termogravimetrijska analiza pokazali da su produkti svih etiriju reakcija jednaki, nije raena kvantitativna analiza ugljika, duaika i vodika svih produkata, ve samo onog prireenog s D,L-metioninom. Uzorak je ozra en UV-zra enjem, te mu je nakon toga snimljen EPR spektar. 3.2.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom, D,L-alaninom i morfolinom pri povienoj temperaturi Metanolnoj otopini (20 cm3) diklorodioksomolibdena(VI) (0,5 g, 2,51 mmol) i D,L- metionina (0,094 g, 0,628 mmol) u reakcijskoj tikvici dodana je 10 % otopina morfolina do po etka talo~enja produkta. Reakcijska tikvica spojena je na Liebigovo hladilo (slika 26) i sadr~aj je grijan 2 h na 60 C. Pri tome je tikvica zaatiena od svjetla aluminijskom folijom zbog mogue fotoosjetljivosti spoja. Po zavraetku grijanja, produkt je ostavljen stajati par dana u otopini. Filtracijom i ispiranjem s metanolom dobiveno je 0,48 g ( = 86 %) bijelog produkta. Kvantitativno je odreen sadr~aj molibdena kemijskom i termogravimetrijskom analizom, snimljen IR spektar, rentgenogram praha te je napravljen kvalitativni test na kloride. Analogno je izvedena sinteza i identifikacija s aminokiselinom D,L-alaninom.  Slika  SEQ Slika \* ARABIC 26: Aparatura za reakciju diklorodioksomolibdena(VI) s aminokiselinama D,L-metioninom i D,L-alaninom pri povienoj temperaturi. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.2.3. Prekristalizacija polioksomolibdata(VI) s D,L-metioninom i morfolinom iz vode Produkt dobiven reakcijom diklorodioksomolibdena(VI), D,L-metionina i morfolina u metanolu pri sobnoj temperaturi prekristaliziran je iz vode pri sobnoj temperaturi i pri temperaturi 0 4 C. Zbog slabe topljivosti spoja u vodi (~ 0,2 g u 25 cm3 H2O), vrijeme prekristalizacije morfolinskog produkta bilo je oko 20 dana. Izoliranom produktu bijele boje (m = 0,39 g,  = 79 %) snimljen je IR spektar i rentgenogram praha. Uzorak je ozra en UV-zra enjem, te mu je nakon toga snimljen EPR spektar. Sadr~aj molibdena kvantitativno je odreen kemijskom i termogravimetrijskom analizom te je odreen sadr~aj ugljika, vodika i duaika. Napravljen je i kvalitativni test na kloride. 3.3. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom Namjera je bila provjeriti utjecaj talo~nog reagensa na vrstu i strukturu izoliranog spoja. Stoga su izvedene reakcije s trietilaminom kao kompleksnim kationom u analognim uvjetima kao reakcije s morfolinom. 3.3.1. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom pri sobnoj temperaturi U 10 cm3 metanola otopljeno je 0,25 g diklorodioksomolibdena(VI) (n = 1,26 mmol), dodano je 0,047 g D,L-metionina (n = 0,628 mmol) te je dodana 10 % otopina trietilamina u metanolu. Nakon tri dana iz otopine su filtracijom izdvojeni ~uto-zeleni kristali (m = 0,12 g,  = 26 %) koji su isprani metanolom te im je snimljen IR spektar. Napravljena je termogravimetrijska analiza sadr~aja molibdena. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.3.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i trietilaminom pri povienoj temperaturi Metanolnoj otopini diklorodioksomolibdena(VI) (m = 0,25 g, n = 1,26 mmol u 10 cm3) i 0,047 g D,L-metionina (n = 0,628 mmol) dodana je 10 % otopina trietilamina u metanolu. Reakcijska smjesa zagrijavana je na 60 C, 2 h uz povratno vodeno hladilo (slika 26). Reakcijska tikvica zaatiena je folijom od svjetlosti. Nakon zagrijavanja, otopina je uparena na vakuumu da bi se potaknula kristalizacija zasienjem. Otopina je pri tome postala zelene boje. Nakon 38 dana iz otopine je izolirana smjesa bezbojnih i ~utih kristala. Kristali su razdvojeni mehani ki pod mikroskopom te im je snimljen IR spektar. Ostatak smjese kristala prekristaliziran je iz metanola pri emu su se ~uti kristali otopili, a bezbojni kristali su zaostali u otopini. 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Kemijsku analizu nije bilo mogue provesti jer su reakcijski prinosi bili mali te je prilikom prekristalizacije doalo do potpunog raspada prvotno bezbojnih kristala (tamnoplavo obojenje). 3.4. Reakcija diklorodioksomolibdena(VI) s D,L- metioninom i -pikolinom }eljelo se joa provjeriti koji je utjecaj bazi nosti talo~nog reagensa na strukturu izoliranog polioksomolibdata, tj. derivata s aminokiselinama. U tu svrhu provedene su reakcije analogne dosadaanjima s time da je kao talo~ni reagens koriaten -pikolin. 3.4.1. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i g-pikolinom pri sobnoj temperaturi Otopini diklorodioksomolibdena(VI) (m = 0,25 g, n = 1,26 mmol) i 0,047 g D,L- metionina u metanolu (10 cm3) dodana je 10 % otopina -pikolina u metanolu. Pri tome je doalo do talo~enja bijelog produkta. Drugi dan iz otopine su izolirani kristali (m = 0,16 g,  = 58 %) te su isprani s metanolom. Produktu je snimljen IR spektar, a kemijskom i termogravimetrijskom analizom odreen je sadr~aj molibdena. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.4.2. Reakcija diklorodioksomolibdena(VI) s D,L-metioninom i g-pikolinom pri poviaenoj temperaturi Otopini diklorodioksomolibdena(VI) (0,25 g) i 0,047 g D,L-metionina (n = 0,628 mmol) u metanolu (10 cm3) dodana je 10 % otopina -pikolina u metanolu. Pri tome je doalo do talo~enja bijelog produkta. Reakcijska smjesa zagrijavana je na 60 C, 2 h uz povratno vodeno hladilo (slika 26) i pri tome je reakcijska tikvica zaatiena folijom od svjetlosti. Prilikom zagrijavanja doalo je do potpunog raspada produkta i nastanka plave, ljepljive smjese koja nije identificirana. 3.5. Reakcije diklorodioksomolibdena(VI) s organskim bazama:g-pikolinom, trietilaminom i morfolinom 3.5.1. Reakcija diklorodioksomolibdena(VI) s g-pikolinom pri sobnoj temperaturi Otopini diklorodioksomolibdena(VI) (0,5 g, 2,51 mmol) u metanolu (10 cm3) dodana je 10 % otopina -pikolina u metanolu. Pri tome je talo~io bijeli produkt. Reakcijska tikvica, zaatiena od svjetlosti crnom folijom, ostavljena je stajati tri dana. Iz otopine su izolirani igli asti, bijeli kristali koji rastu iz jednog centra (m = 0,21 g,  = 80 %) te su isprani metanolom. Produktu je snimljen IR spektar te je odreen sadr~aj molibdena termogravimetrijskom i kemijskom analizom. 3.5.2. Reakcija diklorodioksomolibdena(VI) i trietilamina pri sobnoj temperaturi Otopini diklorodioksomolibdena(VI) u metanolu (0,25 g u 10 cm3) dodana je 10 % otopina trietilamnina u metanolu. Reakcijska tikvica zaatiena je od svjetlosti crnom folijom. Nakon etiri dana iz otopine su izolirani ~uto-zeleni kristali te su isprani s metanolom. Dobivenom produktu snimljen je IR spektar. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.5.3. Reakcija diklorodioksomolibdena(VI) i morfolina pri sobnoj temperaturi Metanolnoj otopini diklorodioksomolibdena(VI) (m = 0,5 g, n = 2,51 mmol u 20 cm3) dodana je 10 % otopina morfolina u metanolu pri emu je doalo do talo~enja bijelog produkta. Reakcijska smjesa zaatiena je crnom folijom od svjetlosti zbog mogue fotoosjetljivosti spoja i ostavljena stajati par dana. Filtracijom uz ispiranje s metanolom izoliran je bijeli, praakasti produkt (0,49 g,  = 96 %) koji je slabo topljiv u vodi i metanolu, a stajanjem i pod utjecajem svjetlosti poprima plavu boju. Produktu je snimljen IR spektar, kvantitativno odreen sadr~aj molibdena kemijskom i termogravimetrijskom analizom, odreen je sadr~aj ugljika, vodika i duaika, snimljen rentgenogram praha i napravljen kvalitativni test na kloride. Uzorak je ozra en UV-zra enjem, te mu je nakon toga snimljen EPR spektar. 3.5.4. Reakcija diklorodioksomolibdena(VI) i morfolina pri poviaenoj temperaturi Metanolnoj otopini diklorodioksomolibdena(VI) (m = 0,5 g, n = 2,51 mmol u 10 cm3) u reakcijskoj tikvici dodana je 10 % otopina morfolina u metanolu pri emu je trenutno talo~io bijeli produkt. Tikvica je spojena na povratno vodeno hladilo (slika 26) i zagrijavana 2 h na 60 C te je pri tom zaatiena aluminijskom folijom od svjetlosti. Nakon dva dana filtriranjem, ispiranjem s metanolom izoliran je bijeli, praakasti produkt (0,25 g,  = 89 %). Napravljen je kvalitativni test na kloride, sadr~aj molibdena odreen je kemijskom i termogravimetrijskom analizom, snimljen je IR spektar te rentgenogram praha izoliranog produkta. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.6. Metode identifikacije izoliranih produkata Da bi se izoliranim produktima odredila fizikalno  kemijska svojstva i odredio molekulski sastav, provedene su analize: kemijska analiza sadr~aja molibdena, kvalitativni test na kloride, kemijska analiza sadr~aja ugljika, vodika i duaika, termogravimetrijsko odreivanje sadr~aja molibdena, infracrvena spektroskopija, UV-ozra ivanje, elektronska paramagnetska rezonancija i difrakcija rentgenskih zraka na polikristalnom uzorku. 3.6.1. Kemijska analiza sadr~aja molibdena Uzorak kompleksa (oko 0,1 g) odvagan je na analiti koj vagi u visoku aau. Razaranje kompleksa vraeno je postupnim dodavanjem konc. p.a. duai ne kiseline u volumenima 2 3 cm3 i istovremenim zagrijavanjem. Kada je uzorak kompleksa razgraen, ato se vidi po pojavi bijelog taloga molibdenovog trioksida, kiselina je uparena do suha i ohlaeni talog otopljen je dodatkom konc. amonijaka te je sve razrijeeno dodatkom 50 cm3 vode. Otopini je podeaen pH = 6 pomou sumporne kiseline (c = 1 mol dm-3) i dodano je 5 cm3 otopine amonijeva acetata (c = 1 mol dm-3). Otopina je zagrijana do vrenja te je potom talo~en molibden 5 % otopinom 8-hidroksikinolina u obliku ~utog, pahuljastog taloga. Dodatkom par kapi otopine 8-hidroksikinolina provjerena je potpunost talo~enja. Nastali talog sastava [MoO2(C9H6ON)2] profiltriran je preko izvaganog G-3 lon ia i ispran s oko 500 cm3 vrue vode ime je uklonjen viaak reagensa. Talog u lon iu suaen je 1 h na 110 C u suaioniku do konstantne mase, ohlaen u eksikatoru i vagan na analiti koj vagi kao bis(8-hidroksikinolato)dioksomolibden(VI), [MoO2(C9H6ON)2]. Iz dobivene mase izra unat je maseni udio molibdena u po etnom kompleksu. 3.6.2. Kvalitativni test na kloride Mala koli ina analita otopljena je u najmanjem volumenu 10 % otopine natrijeve lu~ine, NaOH i zagrijana do vrenja. Dodatkom otopine srebrovog nitrata, AgNO3 (c = 0,5 mol dm-3) talo~en je srebrov oksid, Ag2O. Zakiseljavanjem smjese 10 % otopinom duai ne kiseline, HNO3, talo~e se kloridi. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ Smjesa se zagrije do vrenja i ostavi stajati jedan dan zaatiena od svjetlosti. Ako nastane zamuenje u otopini zbog koloidno raspraenih estica srebrovog klorida, AgCl, u analitu su prisutni kloridi. 3.6.3. Kemijska analiza sadr~aja ugljika, vodika i duaika Sadr~aj ugljika, vodika i duaika odreen je u Institutu Ruer Boakovi. Ugljik i vodik odreeni su spaljivanjem u kisiku, a duaik je odreen Kjeldahl  ovom metodom. 3.6.4. Termogravimetrijsko odreivanje sadr~aja molibdena Termogravimetrijska analiza (TGA) je metoda u kojoj se prati promjena mase uzorka s promjenom temperature u atmosferi nekog plina (O2, N2 Ar, CO2). Promjena temperature u vremenskom intervalu je konstantna. Dobiveni rezultati prikazuju se krivuljom ovisnosti mase o temperaturi i/ili vremenu. Na temelju oblika krivulje zaklju uje se o termi koj stabilnosti uzorka, njegovoj hlapljivosti i moguim putevima termi kog raspada. Na temelju preostale mase oksida nakon spaljivanja uzorka u struji kisika, odreuje se sadr~aj metala u po etnom spoju. Termogravimetrijska analiza je precizna, brza i zahtijeva male koli ine uzorka (g). Nedostatak ove metode jest da je destruktivna ato mo~e biti problem ako je izolirana masa produkta mala. Termogravimetrijska analiza produkata izvedena je na Zavodu za opu i anorgansku kemiju na Mettler TG 15 termovagi. Za spaljivanje izoliranih spojeva koriateni su aluminijski lon ii u atmosferi kisika u temperaturnom podru ju 25  600 C. Svi eksperimenti provedeni su uz zagrijavanje 10 C min-1 i uz protok kisika od 200 cm3 min-1. Rezultati su obraeni primjenom STARe 6.1 programa. Diplomski rad Eksperimentalni dio ___________________________________________________________________________ 3.6.5. Infracrvena spektroskopija Infracrvena spektroskopija esta je metoda identifikacije istih organskih i anorganskih spojeva budui da svaka molekula daje jedinstven i karakteristi an infracrveni spektar. Na temelju usporedbe infracrvenog spektra analita i infracrvenih spektara poznatih analita iz baze podataka, mogua je identifikacija nepoznatog analita. Asignacijom siganala u infracrvenom spektru mogu se predvidjeti funkcionalne skupine analita te na temelju toga pretpostaviti sastav analita. Infracrveni spektri mogu se snimati u sva tri agregatna stanja. vrsti uzorci snimaju se metodom KBr pastile, razmuljivanja u parafinskom ulju ( nujol ) ili pripremom otopine analita (kloroform, tetraklorugljik, ugljikov disulfid). Infracrveni spektri izoliranih spojeva snimljeni su na Zavodu za opu i anorgansku kemiju tehnikom KBr pastile na spektrofotometru FTIR 1600 u podru ju valnih brojeva od 4400 cm-1 do 450 cm-1. 3.6.6. UV-ozra ivanje Izolirani spojevi ozra ivani su u kvarcnim posudicama pod lampom UV  zra enjem valne duljine  = 254 nm i  = 366 nm oko 10 h uzastopce tijekom tri dana. 3.6.7. Elektronska paramagnetska rezonancija Elektronska paramagnetska rezonancija (EPR) je spektroskopska metoda kojom se detektiraju energijski prijelazi spina elektrona u paramagnetskim sustavima u vanjskom magnetskom polju.28 Za postizanje rezonancije i zadovoljenja uvjeta apsorpcije zra enja koristi se mikrovalno i daleko infracrveno zra enje. Metoda je nedestruktivna i mo~e se koristiti i za kvantitativna odreivanja. Prijelazni metali koji posjeduju nesparene elektrone u d-orbitalama pogodni su za EPR prou avanja s time da na EPR parametre bitno utje e okolina metala (ligandi, otapalo). EPR-om se mogu dinami ki i strukturno karakterizirati kompleksi prijelaznih metala s razli itim ligandima u razli itim fizi ko  kemijskim uvjetima (pH, temperatura, otapalo). Diplomski rad Eksperimentalni dio ___________________________________________________________________________ Elekronski paramagnetski spektri polikristalnih, ozra enih uzoraka snimljeni su na instrumentu Varian E-109 Century Line Series, pri 293 K, centralnom polju G = 0,34 T i s 0,1 T airinom polja (engl. field swap), na Institutu Ruer Boakovi u Zagrebu. Uvjet rezonancije postignut je mijenjanjem vanjskog magnetskog polja, izvor kojeg je elektromagnet, uz stalnu frekvenciju mikrovalova. Izvor mikrovalova je klistron koji mo~e generirati frekvencije od 8,8 GHz do 9,6 GHz. Mikrovalovi s valovodom dovode se do rezonantne aupljine koja ima posebnu geometriju tako da je u sredini maksimalno izra~ena magnetska, a minimalno elektri na komponenta mikrovalova. Na tom mjestu apsorpcija mikrovalova je maksimalna kao i homogeno mikrovalno polje. Prethodno prireeni, ozra eni uzorak stavljen je u staklenu kapilaru koja se spuata u rezonantnu aupljinu tako da uzorak bude u sredini iste. Iz EPR spektra odreen je g faktor koji proizlazi iz vrtnje elektrona oko vlastite osi, odnosno magnetskog momenta elektrona. Za slobodni elektron u vakuumu iznosi ge = 2,00232.33 Openito, g faktor je tenzor drugog reda. U otopinama, zbog molekulskih gibanja, anizotropne komponente g  tenzora su usrednjene i dobiva se vrijednost izotropnog g faktora, g0. Sa vrijednoau g faktora povezana je elektronska struktura promatranog paramagnetskog centra. Kristalno polje u krutinama  gasi orbitni doprinos ukupnom magnetskom momentu elektrona, u osnovnom elektronskom stanju. Kako dolazi do meudjelovanja osnovnog s pobuenim elektronskim stanjima u kojima postoji orbitni doprinos, dolazi i do sprezanja spinske i orbitne kutne koli ine gibanja ato se reflektira u odstupanju g faktora od ge. Veina organskih radikala ima g faktor dosta blizak ge, anorganski radikali imaju vrijednosti g faktora od 1,9 do 2,1.34 Prijelazni metali pokrivaju najaire podru je vrijednosti g faktora od 0 do 6 i ovdje g faktor mo~e ukazati na identifikaciju metalnog iona.34 Vrijednost g faktora u molibdenskom enzimu ksantin nitrogenazi za 4d1 elektron pri T<300 K iznosi 1,95-2,0.28 3.6.8. Difrakcija rentgenskih zraka na polikristalnom uzorku Difrakcija rentgenskih zraka na polikristalnom uzorku koristi se za kvalitativnu i kvantitativnu analizu analita, odreivanje parametara jedini ne elije, kristalne i molekulske strukture, veli ine kristalita, prou avanje stresa i strukture materijala. Za metodu difrakcije rentgenskog zra enja na polikristalnom uzorku koristi se monokromatsko, rentgensko Diplomski rad Eksperimentalni dio ___________________________________________________________________________ zra enje, a signali u spektru odgovaraju pojavi difrakcije na mre~nim ravninama u kristalu prema Braggovom zakonu. Kako svaki spoj daje jedinstven difraktogram, difrakcija rentgenskog zra enja na polikristalnom uzorku iskoriatena je kao identifikacijska metoda. Difraktogrami polikristalnih uzoraka snimljeni su na automatskom difraktometru Philips PW1750, a  sirovi podaci sakupljeni su Philips X'Pert programom koji se sastoji od dva modula: X'Pert Data Collector koji slu~i za podeaavanje parametara pokusa i izvoenje mjerenja te modula za prikaz i obradu podataka X'Pert Graphic and Identify. Difraktogram izoliranih spojeva snimljen je na silicijevom nosa u budui da je koli ina analita bila ograni ena. Mjerenja su izvedena na Zavodu za opu i anorgansku kemiju. 4.Rezultati i rasprava   Diplomski rad Rezultati i rasprava ___________________________________________________________________________ 4.1. Identifikacija morfolinijevih polioksomolibdata(VI)  Shema 5: Prikaz provedenih reakcija s morfolinom i dobivenih produkata. [C4H10NO]6[Mo8O26(OCH3)2] Reakcijom diklorodioksomolibdena(VI), aminokiseline (D,L-metionin, D,L-alanin, L-leucin i L-valin) i morfolina u metanolu pri sobnoj temperaturi izoliran je spoj (A) formule [C4H10NO]6[Mo8O26(OCH3)2] (shema 5). Isti produkt dobiven je reakcijom diklorodioksomolibdena(VI), aminokiseline (D,L-metionin, D,L-alanin) i morfolina u metanolu pri poviaenoj temperaturi (60 C) te reakcijom diklorodioksomolibdena(VI) i morfolina bez dodatka aminokiseline pri sobnoj temperaturi (shema 5). Iz IR spektra produkta (A) (dodatak 1a) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 526 (m), 686 (vs), 910 (vs), 1044 (m), 1060 (m), 1106 (s), 1452 (m), 2738 (m), 2806 (m), 2930 (m), 2860 (m), 2980 (m), 3447 (m), (tablica 2). Kemijskom (KA) i termogravimetrijskom (TG) analizom (dodatak 2a) dobiveni su sljedei podaci: w(Mo)KA = 42,78 %, w(Mo)TG = 43,07 %, w(C) = 17,51 %, w(N) = 4,25 %, w(H) = 3,25 %. Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. Iz provedene TG analize o itana su dva koraka raspada, prvi u kojem gubitak mase odgovara masi vezanih metokso skupina zajedno s masom odgovarajueg kompleksnog kationa i drugi koji odgovara masi preostalog molibdenovog trioksida nakon spaljivanja u kisiku. Ti podaci odgovaraju odreenoj formuli. Diplomski rad Rezultati i rasprava ___________________________________________________________________________ Snimljen je difraktogram praha polikristalnih produkta i IR spektar (A) (dodatak 3a) te je utvreno da su isti za sve spojeve prireene ovim kemijskim reakcijama. Uzorak (A) izlo~en je UV-zra enju pri emu je promijenio boju iz bijele u smeu (slika 27). EPR spektrom potvrena je fotoredukcija (dodatak 4a) te je odreen parametar g = 2,0028. Spoj je fotoosjetljiv i duljim stajanjem dolazi do spontane redukcije. Slabo je topljiv u vodi i metanolu.  Slika 27: Spoj A nakon utjecaja UV zra enja. [C4H10NO]4[Mo8O26]2H2O Prekristalizacijom produkta (A) iz vode dobiva se vrlo fotoosjetljiv, bijeli, igli asti produkt (B) sastava [C4H10NO]4[Mo8O26]2H2O (shema 5). Iz IR spektra produkta (B) (dodatak 1b) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 524 (m), 558 (m), 592 (m), 659 (m), 704 (m), 844 (m), 870 (m), 912 (vs), 945 (vs), 1042 (m), 1091 (m), 1103 (m), 1451 (m), 1584 (m), 2964 (m), 3097 (m), 3147 (m), 3413 (m), 3630 (m), 3651 (m), (tablica 2). Kemijskom analizom (KA) i termogravimetrijskom (TG) analizom (dodatak 2b) dobiveni su sljedei podaci: w(Mo)KA = 47,28 %, w(Mo)TG = 48,20 % , w(C) = 12,45 %, w(N) = 3,16 %, w(H) = 2,71 % (tablica 3 i 4). Iz TG analize produkta [C4H10NO]4[Mo8O26]2H2O o itan je raspad u tri koraka u kojem prvi odgovara izla~enju kristalno vezane vode, drugi korak odgovara raspadu kompleksnog kationa, dok ostatak nakon spaljivanja u kisiku odgovara masi molibdenovog trioksida. Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. Produktu (B) snimljen je i difraktogram praha (dodatak 3b). Djelovanjem UV-zra enja dolazi do promjene boje produkta (B) iz bijele u sivo  plavu ato indicira redukciju Mo(VI) u Mo(V) (slika 28), a ato je i potvreno EPR spektrom (dodatak 4b) iz kojeg je odreen parametar g = 2,0028. Diplomski rad Rezultati i rasprava ___________________________________________________________________________ Prekristalizacijom polioksometoksomolibdata u vodi dolazi do disocijacije koordiniranih metokso skupina i nastanka oktamolibdata koji je vjerojatno je -izomer sa strukturom analognoj spoju sastava [C4H10NO]4[Mo8O26]4H2O opisanom u literaturi.21  Slika 28: Spoj B nakon utjecaja UV zra enja. [C4H10NO]4[Mo8O24(OCH3)4] Reakcijom diklorodioksomolibdena(VI) i morfolina u metanolu pri sobnoj temperaturi dobiven je bijeli, polikristalan spoj (C), [C4H10NO]4[Mo8O24(OCH3)4] (shema 5). Iz IR spektra produkta (C) (dodatak 1c) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 520 (m), 553 (m), 698 (m), 852 (m), 871 (m), 913 (vs), 941 (vs), 1035 (m), 1105 (m), 1451 (m), 1592 (m), 2478 (m), 2860 (m), 2972 (m), 3080 (m), 3240 (m), 3478 (m), 3650 (m), 3678 (m), (tablica 2). Kemijskom analizom (KA) i termogravimetrijskom (TG) analizom (dodatak 2c) dobiveni su sljedei podaci: w(Mo)KA = 46,55 %, w(Mo)TG = 46,99 %, w(C) = 14,23 %, w(N) = 3,11 %, w(H) = 3,45 % (tablica 3 i 4). Iz provedene TG analize o itana su dva koraka raspada u kojima gubitak mase odgovara masi vezanih metokso skupina zajedno s masom odgovarajueg kompleksnog kationa i ostatku molibdenovog trioksida nakon spaljivanja u kisiku. Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. Produktu (C) snimljen je i difraktogram praha (dodatak 3c) te je izlo~en UV-zra enju pod ijim utjecajem mijenja boju iz bijele u plavu (slika 29). Fotoredukcija je potvrena EPR spektrom (dodatak 4c) iz kojeg je odreen i parametar g = 2,0028.  Slika 29: Spoj C nakon djelovanja UV zra enja. Diplomski rad Rezultati i rasprava ___________________________________________________________________________ Prou avanjem izoliranih morfolinijevih produkata vidljivo je da dolazi do koordinacije dvije ili etiri metokso skupine na oktamolibdatnu jezgru. Iz literaturnih izvora1 mo~e se zaklju iti da su to derivati izomera -[Mo8O26]4- u kojima su dvije metokso skupine premoaujue, a dvije terminalne te da je svaki Mo-atom oktaedarski koordiniran s O-donorskim ligandima (slika 15).1 Poznati su navodi iz literature koji dokazuju da koordinirane metokso skupine prelaze u formaldehid, oktamolibdat i vodu pri TG analizi u temperaturnom podru ju do 500 C, prilikom bla~eg zagrijavanja ili izlaganja svjetlosti.26 Razli itost difraktograma praha izoliranih morfolinijevih polioksometoksomolibdata(VI) dokaz su razli itog sastava i pretpostavljene strukture. Diplomski rad Rezultati i rasprava ___________________________________________________________________________ 4.2. Identifikacija trietilamonijevih polioksomolibdata(VI)  Shema 6: Prikaz provedenih reakcija s trietilaminom i dobivenih produkata. [(C2H5)3NH]2[MoO4] Reakcijom diklorodioksomolibdena(VI), D,L- metionina i trietilamina u metanolu pri sobnoj temperaturi, izolirani su igli asti, ~uto-zeleni kristali (D) sastava [(C2H5)3NH]2[MoO4] (shema 6). Isti spoj dobiven je reakcijom diklorodioksomolibdena(VI) i trietilamina u metanolu pri sobnoj temperaturi te reakcijom diklorodioksomolibdena(VI), D,L-metionina i trietilamina u metanolu pri poviaenoj temperaturi kao nusprodukt (shema 6). Iz IR spektra produkta (D) (dodatak 1d) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 804 (s), 955 (s), 1457 (m), 1472 (m), 3030 (m), 3165 (m), 3463 (m), (tablica 2). Termogravimetrijskom (TG) analizom (dodatak 2d) dobiveni su sljedei podaci: w(Mo)TG = 26,81 % (tablica 3 i 4). Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. Trietilamonijev oktamolibdat Reakcijom diklorodioksomolibdena(VI), D,L-metionina i trietilamina u metanolu pri poviaenoj temperaturi dobivena je smjesa bezbojnih i ~utih kristala (shema 6). IR spektar ~utih kristala odgovara produktu (D), dok IR spektar bezbojnih kristala odgovara trietilamonijevom oktamolibdatu (E) (dodatak 1e). Diplomski rad Rezultati i rasprava ___________________________________________________________________________ Iz IR spektra produkta (E) (dodatak 1e) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 523 (m), 557 (m), 659 (s), 707 (s), 734 (s), 842 (s), 907 (vs), 940 (vs), 1252 (m), 1392 (m), 1469 (m), 1484 (m), 2800 (m), 3031 (m), 3126 (m), 3494 (m), (tablica 2). Bezbojni kristali vrlo su fotosenzibilni. Zbog raspada produkta (E), analize sastava spoja nisu provedene. Dodavanjem trietilamina u reakcijsku smjesu nije doalo do trenutnog talo~enja produkta kao kod ostalih provedenih reakcija, ve je produkt izoliran tek nakon duljeg stajanja u otopini. Vjerojatno zbog dugog stajanja, iz otopine je izoliran trietilamonijev molibdat. Trietilamonijev oktamolibdat identificiran je na temelju signala u IR spektru karakteristi nih za oktamolibdatnu jezgru (Mo-Ot i Mo-O-Mo), a prireen je u uvjetima (poviaena temperatura) sli nim nastanku spoja sastava [Et3NH]4[Mo8O26] opisanog u literaturi.35 Trietilamonijev okatmolibdat [Et3NH]4[Mo8O26] prema literaturi, pripremljen je reakcijom trietilamina i molibdenovog trioksida ili amonijevog molibdata u vodenoj otopini klorovodi ne kiseline, refluksiranjem tijekom 24 h istalo~en je oktamolibdat za koji je utvrena polimerna struktura graena od -izomera oktamolibdata.35 Diplomski rad Rezultati i rasprava ___________________________________________________________________________ 4.3. Identifikacija -pikolinskih polioksomolibdata(VI)  Shema 7: Prikaz provedenih reakcija s -pikolinom i dobivenih produkata. [C6H8N]4[Mo8O24(OCH3)4] Reakcijom diklorodioksomolibdena(VI) i -pikolina u metanolu pri sobnoj temperaturi dobiven je bijeli produkt (F) sastava [C6H8N]4[Mo8O24(OCH3)4] (shema 7). Iz IR spektra produkta (F) (dodatak 1f) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 486 (m), 525 (m), 569 (m), 683 (m), 891 (m), 913 (s), 935 (m), 984 (m), 1017 (m), 1053 (m), 1502 (m), 1635 (m), 2815 (m), 2935 (m), 2990 (m), 3071 (m), 3432 (m), (tablica 2). Kemijskom analizom (KA) i termogravimetrijskom (TG) analizom (dodatak 2e) dobiveni su sljedei podaci: w(Mo)KA = 46,67 %, w(Mo)TG = 47,32 % (tablica 3 i 4). Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. [C6H8N]4[Mo8O24(OCH3)4]3CH3OH Reakcijom diklorodioksomolibdena(VI) i -pikolina u metanolu pri sobnoj temperaturi dobiven je bijeli produkt (G) sastava [C6H8N]4[Mo8O24(OCH3)4]3CH3OH (shema 7). Iz IR spektra produkta (F) (dodatak 1g) mogu se izdvojiti sljedei karakteristi ni valni brojevi:  EMBED Equation.3 /cm-1 = 476 (m), 518 (m), 560 (m), 641 (m), 665 (m), 680 (m), 795 (m), 849 (m), 903 (s), 917 (m), 933 (m), 1506 (m), 1618 (m), 1637(m), 3079 (m), (tablica 2). Diplomski rad Rezultati i rasprava ___________________________________________________________________________ Kemijskom analizom (KA) i termogravimetrijskom (TG) analizom (dodatak 2f) dobiveni su sljedei podaci: w(Mo)KA = 44,17 %, w(Mo)TG = 43,97 % (tablica 3 i 4). Iz TG krivulje za produkt [C6H8N]4[Mo8O24(OCH3)4]3CH3OH o itana su dva koraka raspada koji upuuju na razli ito vezani metanol (kristalno i kompleksno). Kvalitativnim testom na kloride utvreno je da u spoju nije prisutan klor. Mo~e se pretpostaviti da su -pikolinski produkti derivati -izomera oktamolibdata(VI) u kojem su metokso skupine terminalne i premoaujue, analogno kao u morfolinijevim produktima. Polioksometoksomolibdati(VI) s -pikolinom dosada nisu opisani u literaturi, a najsli niji opisani produkti su oni s piridinom i N-metilpiridinom. Iz navedenih primjera vidljiv je utjecaj i najmanje promjene reakcijskih uvjeta na strukturu izoliranog produkta i poteakoa pri bilo kakvoj sistematizaciji ili predvianju strukture produkta. Diplomski rad Rezultati i rasprava ___________________________________________________________________________ 4.4. Identifikacija produkata infracrvenom spektroskopijom Za oktamolibdate: vibracija (Mo-Ot) o ekuje se oko 940 cm-1 i odgovara simetri nom istezanju Mo-Ot veze, dok se asimetri no istezanje o ekuje oko 915 cm-1; vibracija (Mo-O-Mo) o ekuje se oko 700 cm-1.36 Kristalno vezana voda apsorbira u podru ju od 3550-3200 cm-1 (antisimetri na i simetri na vibracija istezanja O-H veze).37 Vibracije C-O veze u metokso skupini nalazimo u podru ju 875-1100 cm-1.36 U podru ju 3000-2860 cm-1, 1470-1400 cm-1, 1380-1200 cm-1 i 1200-800 cm-1 o ekuje se vibracija C-H veze iz metokso skupine i C-H veze iz kationa (morfolin, -pikolin, trietilamin).37 U slu aju koordinirane aminokiseline, u IR spektru vidljiva je airoka i jaka apsorpcija u podru ju 3100-2600 cm-1 uzrokovana istezanjem N H veze amino skupine te vrpce u intervalu 2222-2000 cm-1; u podru ju 1660-1610 cm-1 opa~a se slaba vrpca uzrokovana antisimetri nim istezanjem N H veze amino skupine i jaka vrpca oko 1550-1485 cm-1 uzrokovana simetri nim istezanjem iste; karboksilatni ion jako apsorbira pri 1600-1530 cm-1 i mnogo slabije u blizini 1400 cm-1.37 /cm-1686 909, 936 871 704 912, 945 3147, 3413 698 913, 941 871, 897 804, 955  707 907, 940  683 913, 935 891 680 903, 917, 933 849 vibracija vezeMo-O-Mo Mo-Ot C-OMo-O-Mo Mo-Ot H2O  Mo-O-Mo Mo-Ot C-O  Mo-Ot  Mo-O-Mo Mo-Ot Mo-O-Mo Mo-Ot C-O  Mo-O-Mo Mo-Ot C-O /cm-1526(m), 574 (m), 686 (vs), 871 (vs), 909 (vs), 936 (s), 990 (s), 1044 (m), 1060 (m), 1106 (s),1156 (w), 1191 (w),1235 (w), 1303 (w), 1354 (vw), 1378 (wv), 1398 (w), 1427 (w), 1452 (m), 1604 (m), 2200(vw), 2461 (m), 2738 (m), 2806 (m), 2860 (m), 2930 (m), 2980 (m), 3447 (m)481 (m), 524 (m), 558 (m), 592 (m), 659 (m), 704 (m), 795 (m), 844 (m), 870 (m), 912 (vs), 945 (vs), 1023 (w),1042 (m), 1091 (m), 1103 (m), 1187 (vw), 1233 (vw), 1315 (w), 1376 (w), 1451 (m), 1499 (vw), 1508 (vw),1584 (m),1637 (w), 1654 (w), 1686 (vw), 1701 (vw), 1719 (vw), 2345 (m), 2365 (m), 2464 (m), 2964 (m), 3097 (m), 3147 (m), 3413 (m), 3630 (m), 3651 (m), 3678 (w), 3736 (w), 3840 (w), 3855 (w)520 (m), 553 (m), 698 (m), 852 (m), 871 (m), 897 (m), 913 (vs), 941 (vs), 1035 (m), 1105 (m), 1153 (vw), 1191 (w), 1231 (vw), 1310 (w), 1404 (w), 1451 (m), 1499 (w), 1592 (m), 1654 (w), 1686 (vw, br), 1702 (vw), 1719 (vw), 2346 (w), 2478 (m), 2860 (m), 2972 (m), 3080 (m), 3240 (m), 3478 (s), 3650 (m), 3678 (m), 3691(w),3713 (w), 3736 (w), 3840 (w), 3855 (w)596 (w), 668 (w), 804 (s), 955 (s), 1011 (w), 1031 (w), 1058 (vw), 1175 (w), 1287 (w), 1399 (m), 1457 (m), 1472 (m),1507 (wv), 1559 (vw), 1636 (w), 1653 (w), 1700 (vw), 2343 (w), 2362 (w), 2706 (w), 2809 (w), 3030 (m), 3165 (m),3436 (m), 3676 (w), 3751 (w), 3854 (w)475 (m), 523 (m), 557 (m), 659 (s), 707 (s), 734 (s), 842 (s), 907 (vs), 940 (vs), 1032 (w), 1072 (vw), 1184 (vw), 1212 (w), 1252 (m), 1290 (vw), 1313 (vw), 1392 (m), 1469 (m), 1484 (m), 1588 (vw), 1654 (vw),1754 (m), 2800 (m), 3031 (m), 3126 (m), 3494 (m)486 (m), 525 (m), 569 (m), 683 (m), 805 (w), 828 (w), 845 (w), 891 (m), 913 (s), 935 (m), 984 (m), 1017(m), 1053 (m), 1147 (vw), 1203 (w), 1256 (vw), 1321 (vw), 1388 (w), 1445 (w), 1502 (m), 1528 (vw), 1635 (m), 2006 (w), 2119 (w), 2815 (m), 2935 (m), 2990 (m), 3071 (m), 3432 (m)476 (m), 518 (m), 560 (m), 604 (m), 641 (m), 665 (m), 680 (m), 795 (m), 818 (w), 849 (m), 903 (s), 917 (m), 933 (m), 1004 (vw), 1035 (w), 1075 (w), 1201 (w), 1255 (vw), 1321 (vw), 1376 (vw), 1443 (vw), 1506 (m), 1618 (m), 1637 (m), 2080 (vw), 2344 (w), 2366 (w), 2802 (w), 3079 (m), 3220 (w), 3465 (w)produktABCDEFGDiplomski rad Rezultati i rasprava ___________________________________________________________________________ Diplomski rad Rezultati i rasprava ___________________________________________________________________________ 4.5. Identifikacija produkata termogravimetrijskom i kemijskom analizom % Mo opa~eni (ra unani)43,07 (43,26)48,20 (48,82)46,99 (47,14)26,81 (26,33)47,32 (46,46)43,97 (43,91)% MoO3 nakon spaljivanja opa~eni (ra unani)64,62 (64,89)72,31 (73,25)70,28 (70,72)40,21 (39,49)70,98 (69,69)65,95 (65,85)ukupni gubitak mase (%) opa~eni (ra unani)35,38 (35,11)27,69 (26,76)29,72 (29,28)59,47 (60,50)29,03 (30,31)34,01 (34,14 )raspad ( C)179 - 384 384 - 428260 - 396 410 - 43425 - 144 143 - 385 402 - 432179 - 253 260 - 471 69 - 52097 - 259 259 - 458 gubitak mase (%) opa~eni (ra unani)2,69 (2,29)gubitak otapala ( C)30-117Kompleks[C4H10NO]6[Mo8O26(OCH3)2] (A)[C4H10NO]4[Mo8O26]2H2O (B)[C4H10NO]4[Mo8O24(OCH3)4] (C)[(C2H5)3NH]2[MoO4] (D)[C6H8N]4[Mo8O24(OCH3)4] (F)[C6H8N]4[Mo8O24(OCH3)4] 3CH3OH (G) Diplomski rad Rezultati i rasprava ___________________________________________________________________________ KAr.p./ %10,31,049,6---w(N)/% r.4,743,563,44---w(N) /%4,253,613,11---r.p./ %0,130,0280,068---w(H)/% r.3,752,833,23---w(H)/%3,252,913,45---r.p./ %0,511,9 3,5---w(C)/% r.17,612,2214,75---w (C)/%17,5112,4514,23---r.p./ %1,13,21,3-0,430,59w(Mo) /%42,7847,2846,55-46,6744,17TGr.p./ %0,391,30,321,91,80,14w(Mo)/% r.43,2648,8247,1426,3346,4643,91w (Mo)/%43,0748,2046,9926,8147,3243,97Kompleks[C4H10NO]6[Mo8O26(OCH3)2] (A)[C4H10NO]4[Mo8O26]2H2O (B)[C4H10NO]4[Mo8O24(OCH3)4] (C)[(C2H5)3NH]2[MoO4] (D)[C6H8N]4[Mo8O24(OCH3)4] (F) [C6H8N]4[Mo8O24(OCH3)4] 3CH3OH (G)   5. Zaklju ak   Diplomski rad Zaklju ak ___________________________________________________________________________ Istra~ivanje u ovom diplomskom radu odnosi se na ispitivanje uvjeta nastajanja polioksomolibdata(VI) s organskim ligandima (aminokiseline, metanol) kao i na njihovu izolaciju te identifikaciju. Nastojalo se prirediti derivate -izomera oktamolibdata s aminokiselinama: D,L-metioninom, D,L-alaninom, L-leucinom i L-valinom uz dodatak organskih baza (morfolin, trietilamin, -pikolin). Meutim, izolirani produkti identificirani su kao polioksometoksomolibdati(VI), bez utjecaja dodane aminokiseline: Reakcijom diklorodioksomolibdena(VI) i morfolina u metanolu pri sobnoj i poviaenoj temperaturi dobiveni su morfolinijevi polioksometoksomolibdati i morfolinijev oktamolibdat nakon prekristalizacije iz vode: [C4H10NO]6[Mo8O26(OCH3)2], [C4H10NO]4[Mo8O24(OCH3)4], [C4H10NO]4[Mo8O26]2H2O. Reakcijom diklorodioksomolibdena(VI) i trietilamina u metanolu pri sobnoj temperaturi nastaje: [Et3NH]2[MoO4], a pri poviaenoj nastaje trietilamonijev oktamolibdat. Reakcijom diklorodioksomolibdena(VI) i -pikolina u metanolu pri sobnoj temperaturi nastaju polioksometoksomolibdati: [C6H8N]4[Mo8O24(OCH3)4]3CH3OH, [C6H8N]4[Mo8O24(OCH3)4]. Istom reakcijom pri poviaenoj temperaturi dolazi do raspada produkta. Na temelju identificiranih spojeva mo~e se zaklju iti i pretpostaviti sljedee: Izolirani spojevi svrstavaju se u polioksoalkoksomolibdate(VI) koji u vodenom mediju nisu stabilni i hidrolizom metokso skupina prelaze u oktamolibdat. Izolirani spojevi derivati su -izomera oktamolibdata u kojima je Mo(VI) koordiniran s dvije ili etiri metokso skupine preko O-atoma. Metokso skupine su terminalne (Mo-OCH3) ili premoaujue (Mo-OCH3-Mo). Stabilnost oktamolibdatne jezgre je velika. Navedeni uvjeti ne pogoduju zamjeni okso skupina oktamolibdata s aminokiselinama, ve pogoduju zamjeni s metokso skupinama. Metokso skupina preferirani je ligand za Mo(VI) te su polioksometoksomolibdati(VI) stabilniji u odnosu na potencijalne komplekse s aminokiselinom u navedenim reakcijskim uvjetima. 6. Literaturni izvori   Diplomski rad Literaturni izvori ___________________________________________________________________________ B. Kamenar, B. Korpar-Colig, M. Penavic, M. Cindric, J. Chem. Soc,. Dalton trans., 1 (1990) 1125-1130. M. Inoue, T. Yamase, Bull. Chem. Soc. Jpn., 68 (1995) 3055-30. D. Grdenic, Povijest kemije, Novi Liber, `kolska knjiga, Zagreb, 2001, str. 480, 482, 560. F. A. Cotton, G. A. Willkinson, Advanced Inorganic Chemistry, 5th ed., John Wiley and Sons, New York, 1998. Introduction in: Chem. Rev., 98 (1998). X. L. Fernndez, Theoretical Study of the Basicity and the Redox Properties of Heteropolyanions, Universitat Rovira i Virgili, Tarragona, 2003. D. E. Katsoulis, Chem. Rev., 98 (1998) 359-387. D. H. Killeffer, A. Linz, Molybdenum Compounds: their chemistry and technology, Interscience Publishers, New York, 1952, str. 41-45, str. 111-115. H. Fujita, T. Fujita, T. Sakurai, T. Yamase, Y. Seto, Tohoku J. Exp. Med., 168(2) (1992) 421-426. Y. Inouye, Y. Tokutake, T. Yoshida, Y. Seto, H. Hujita, K. Dan, A. Yamamoto, S. Nishiya, T. Yamase, S. Nakamura, Antiviral Res., 20(4) (1993) 317-331. L. C. W. Baker, D. G. Glick, Chem. Rev., 98 (1998) 3-49. M. T. Pope, Isopolyanions and Heteropolyanions, u: G. Wilkinson, R. D. Gillard, J.A. McCleverty, Comprehensive Coordination Chemistry, Vol. 3, Pergamon Press, 1982, 1023-1058. N. Hall, Chem. Commun., 7 (2003) 803-806. O. Nagano, Y. Sasaki, Acta Crystallogr., Sect. B, 35 (1979) 2387. I. Knoepnadel, H. Hartl, W. D. Hunnius, J. Fucs, Angew. Chem., Int. Ed. Engl., 13 (1974) 823. V. W. Day, M. Frederich, W. G. Klemperer, W. Shum, J. Am. Chem. Soc., 99 (1977) 6146. L.-K. Yan, Z.-M. Su, W. Guan, M. Zhang, J. Phys. Chem. B, 108 (2004) 17337-17343. C.-C. Jiang, G. Liu, Y.-G. Wei, W. Wang, S.-W. Zhang, Inorganic Chemistry Commu., 2 (1999) 258-260. P. Gili, P. A. L. Louis, A. Mederes, J. A. M. Arrieta, G. Germain, A. Castinieras, R. Carballo, Inorg. Chim. Acta, 295 (1999) 106. J. Fuchs, H. Hartl, Angew. Chem., Int. Ed. Engl., 15 (1976) 375. B. Kamenar, M. Penavic, B. Korpar-Colig, M. Cindric, Zeitschrift fr Kristallographie, 210 (1995) 535. P. Gouzerh, A. Proust, Chem. Rev., 98 (1998) 77-111. S. H. Laurie, Amino Acids, Peptides and proteins, u: G. Wilkinson, R. D. Gillard, J.A. McCleverty, Comprehensive Coordination Chemistry, Vol. 2, Pergamon Press, 1982, str. 739-745, 749, 750. Diplomski rad Literaturni izvori ___________________________________________________________________________ J. T. Rhule, C. L. Hill, D. A. Judd, Chem. Rev., 98 (1998) 327-357. N. Mizuno, M. Misono, Chem. Rev., 98 (1998) 199-217. E. M. McCarron, R. L. Harlow, J. Am. Chem. Soc., 105 (1983) 6179-6181. T. Yamase, Chem. Rev., 98 (1998) 307-325. L. Que Jr., Physical Methods in Bioinorganic Chemistry  Spectroscopy and Magnetism, University Science Books, Suasalito, California, 2000, str. 17-28, 121-170. Y. Zhu, Transmission electron microscopy and flow field-flow fractionation: exploration of the nanoscopic components in partially reduced polyoxomolybdates by kinetic precipitation with de novo organic molecules, Lexington, Kentucky, 2003.  HYPERLINK "http://www.chem.uky.edu/research/cammers/theses_pdf/zhu.thesis/yan_zhu_Thesis" http://www.chem.uky.edu/research/cammers/theses_pdf/zhu.thesis/yan_zhu_Thesis (28.02.2005.).  HYPERLINK "http://cmpweb.ameslab.gov/magnetic_molecules/chemprojects.htm#sec1" http://cmpweb.ameslab.gov/magnetic_molecules/chemprojects.htm#sec1 (28.02.2005.). E. Beckman, Synthese neuartiger nanoskalierter Polyoxomolybdat-Cluster, Fakultt fr Chemie der Universitt Bielefeld, 2003.  HYPERLINK "http://bieson.ub.uni-bielefeld.de/volltexte/2004/441/" http://bieson.ub.uni-bielefeld.de/volltexte/2004/441/ (28.02.2005.) A. Mller, M. T. Pope, D. Gatteschi, Chem. Rev., 98 (1998) 239-271. A. Schwiger, G. Jeschke, Principles of Pulse electron paramagnetic resonance, John Wiley and Sons, New York, 1990. P. Atkins, Physical chemistry, Oxford University Press, New York, 1998, str. 557-563. M. McCann, M. Covery, V. Quillet, Polyhedron, 13 (1994) 835-840. M. Cindri, Doktorska disertacija, Zagreb, 1991. Z. Popovi, Infracrvena spektroskopija, Interna skripta, Zagreb, PMF, 1999. Cambridge Structural Database. 7. Kratice    L-METIONIN L-LEUCIN 2-amino-4-(metiltio)butanska kiselina 2-amino-4-metilpentanska kiselina  L-ALANIN L-VALIN 2-aminopropanska kiselina 2-amino-3-metilbutanska kiselina   MORFOLIN -PIKOLIN 1-oksa-azacikloheksan, 4-metilpiridin tetrahidro-1,4-oksazin   L-LIZIN 2,6-diaminoheksanska kiselina flavin mononukleotid Met  metioninato Morph  morfolin MeOH  metanol, CH3OH Et3N - trietilamin OMe - metokso FMN  flavin mononukleotid, 5-fosforiboflavin LMCT  ligand to metal charge transfer CSD  Cambridge Structural Database 8. Dodatak   Diplomski rad Dodatak 1 ___________________________________________________________________________ Dodatak 1a: IR spektar produkta (A), [C4H10NO]6[Mo8O26(OCH3)2].  Dodatak 1b: IR spektar produkta (B), [C4H10NO]4[Mo8O26]2H2O.  Diplomski rad Dodatak 1 ___________________________________________________________________________ Dodatak 1c: IR spektar produkta (C), [C4H10NO]4[Mo8O24(OCH3)4].  Dodatak 1d: IR spektar produkta (D), [(C2H5)3NH]2[MoO4].  Diplomski rad Dodatak 1 ___________________________________________________________________________ Dodatak 1e: IR spektar produkta (E), trietilamonijev oktamolibdat.  Dodatak 1f: IR spektar produkta (F), [C6H8N]4[Mo8O24(OCH3)4].  Diplomski rad Dodatak 1 ___________________________________________________________________________ Dodatak 1g: IR spektar produkta (G), [C6H8N]4[Mo8O24(OCH3)4]3CH3OH.  Diplomski rad Dodatak 2 ___________________________________________________________________________ Dodatak 2a, b, c: TG krivulje produkata [C4H10NO]6[Mo8O26(OCH3)2] (A), [C4H10NO]4[Mo8O26]2H2O (B), [C4H10NO]4[Mo8O24(OCH3)4] (C). Dodatak 2d: TG krivulja produkata (D), [(C2H5)3NH]2[MoO4].  Diplomski rad Dodatak 2 ___________________________________________________________________________ Dodatak 2e: TG krivulja produkata (F), [C6H8N]4[Mo8O24(OCH3)4].  Dodatak 2f: TG krivulja produkata (G), [C6H8N]4[Mo8O24(OCH3)4]3CH3OH. Diplomski rad Dodatak 3 ___________________________________________________________________________ Dodatak 3a: Difraktogram praha produkta (A), [C4H10NO]6[Mo8O26(OCH3)2]. Dodatak 3b: Difraktogram praha produkta (B), [C4H10NO]4[Mo8O26]2H2O.  Diplomski rad Dodatak 3 ___________________________________________________________________________ Dodatak 3c: Difraktogram praha produkta (C), [C4H10NO]4[Mo8O24(OCH3)4].   (C4H10NO)4[Mo8O24(OCH3)4]  (C4H10NO)6[Mo8O26(OCH3)2]  (C4H10NO)4[Mo8O26]2H2O Diplomski rad Dodatak 4 ___________________________________________________________________________ Dodatak 4a: EPR spektar produkta (A), [C4H10NO]6[Mo8O26(OCH3)2].  Dodatak 4b: EPR spektar produkta (B), [C4H10NO]4[Mo8O26]2H2O.  Diplomski rad Dodatak 4 ___________________________________________________________________________ Dodatak 4c: EPR spektar produkta (C), [C4H10NO]4[Mo8O24(OCH3)4].  9. }ivotopis   R oena sam 27.5.1982. godine u akovcu. Nakon zavraene osmoljetke u Kotoribi u kojoj sam provela svoje djetinjstvo, 1996. godine upisala sam srednju Rudarsku i kemijsku akolu u Vara~dinu, smjer kemijski tehni ar. S velikim zanimanjem uklju ila sam se 1998. godine u rad e-akole te sam izradila dva mini-projekta (Izolacija biljnih pigmenata; Izolacija inulina iz korijena masla ka  objavljeni na web stranicama e-akole) s mentorima iz srednje akole i sa znanstvenicima s Instituta Ruer Boakovi, te sam sudjelovala na XVII. Hrvatskom skupu kemi ara i kemijskih tehnologa 1999. godine. Takoer sam dva puta sudjelovala na dr~avnim natjecanjima iz kemije. Sve je to bila dobra priprema za upis na Prirodoslovno-matemati ki fakultet, smjer dipl. ing. kemije 2000. godine. Od tada sam lan Hrvatskog kemijskog druatva te lan Studentske sekcije Hrvatskog kemijskog druatva. Aktivno sam sudjelovala u izvedbama etiri Smotre Sveu iliata. Od 2000. do 2005. g. stipendist sam Ministarstva znanosti, obrazovanja i akolstva. Godine 2004. sudjelovala sam u natje aju za Rektorovu nagradu. PAGE  PAGE ii PAGE 7 Slika  SEQ Slika \* ARABIC 24: Prva objavljena struktura klustera pola u poliedarskom prikazu s razli itim fragmentima  {Mo1}-~uto, {Mo2}-crveno i {Mo8}-plavo (Mo-plavo, O-crveno).13 Slika  SEQ Slika \* ARABIC 2: Jns Jacob Berzelius. (1779. - 1848.) (1779. - 1848.) Slika  SEQ Slika \* ARABIC 12:Ball-and-stick prikaz [Mo6O19]3- strukture.17 Slika  SEQ Slika \* ARABIC 14: Poliedarski prikaz strukture -[Mo8O26]4- izomera.21  EMBED ChemDraw.Document.5.0  Slika  SEQ Slika \* ARABIC 1: Carl Wilhelm Scheele  HYPERLINK "http://www.anoca.org/american/july/1742.html" \o "1742" 1742.-  HYPERLINK "http://www.anoca.org/august/composer/1786.html" \o "1786" 1786.  EMBED ChemDraw.Document.5.0   EMBED ChemWindow.Document  Tablica  SEQ Tablica \* ARABIC 2: Podaci dobiveni infracrvenom spektroskopijom (IR). Tablica 3: Rezulati termogravimetrijske analize (TG). 2980 2930 526 1106 686 910 A 100 % T 30 80 1 70 1452 - -1 / cm-1 50 60 40 2860 90  / m 2806 1044 2738 21 19 17 15 14 13 12 11 10 9 8 7 6 5 4 3 500 1000 1000 1500 2000 4000 3500 3000 2500 2000 1 0,9 0,8 0,7 0,6 0,5 0,4 0,3 0,2 0,1 0 10 20 30 40 50 60 70 80 90 100 20 10 0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1 2000 2500 3000 3500 4000 2000 1500 1000 1000 500 3 4 5 6 7 8 9 10 11 12 13 14 15 17 19 21  / m 80 70 -1 / cm-1 100 % T 90 A 945 704 844 3097 3148 524 3413 1103 1584 550 2964 60 50 40 30 20 10 0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1 2000 2500 3000 3500 4000 2000 1500 1000 1000 500 3 4 5 6 7 8 9 10 11 12 13 14 15 17 19 21  / m 500 450 -1 / cm-1 400 % T 350 A 941 698 3478 553 1105 3080 2972 2860 520 1035 3240 300 250 200 150 100 50 3C min 2 mg 55 50 45 40 35 30 25 20 15 10 5 0 550 500 450 400 350 300 250 200 150 100 50 3C min 10 mg 0 5 10 15 20 25 30 35 40 45 55 mg 2 min 3C 50 100 150 200 250 300 350 400 450 500 550 0 5 10 15 20 25 30 35 40 45 50 55  EMBED ChemWindow.Document   EMBED ChemWindow.Document   EMBED ChemWindow.Document   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0   EMBED ChemDraw.Document.5.0  Tablica 4: Rezultati kemijske analize (KA) i termogravimetrijske analize (TG) s relativnim pogreakama (r.p.) i ra unskim (r.) masenim udjelima pojedinog elementa u izoliranom produktu.  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