“綠色”催化新材料-氮雜環(huán)過渡金屬配位超分子的設計及研究.pdf

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3、yclohexaneoxidationoftransitionmetalsupramolecularcomplexesAbstractCatalyticoxidationofcyclohexane(Cy)hasattractedmuchattentionincatalyticchemistrynemainproductsofCyoxidationarecyclohexanolandcyclohexanone，whichareimport

4、antorganicmaterialsformeproductionofadipicacidandcaprolactum，andfurthersynthesizethenylon一6，6’，nylon一6，polyamide一6，polyurethanefoams，pharmaceuticals，paints，dyesandlubricatingadditivesHowevertherearesomeproblemsintheconve

5、ntionalprocessofCvoxidationsuch嬲muchbyproducts，lowselectivityandemissionsandenvironmentalpollutionTherefore，itisimperativetoseekahighselectivityhighstabilityandenvironmentallyfriendlycatalystInthisthesis，Co(IAA)ffphen)(H

6、20)(1)andNi(IAA)2(phen)(H20)(2)complexesweresynthesizedusingIAAandphen(IAA=indoleaceticacid，phen=l，10一phenanthroline)asligands；ironcomplex[Fe(H2L)2】(CH3COO)2‘(OH)‘H20(3)withH2L(H2L=2，6bis(5一methyl一1H—pyrazol一3一y1)pyridin

7、e)WaSsynthesized；anotherfourcomplexeswithH2LandH2dipic(H2dipic=2，6一pyridinedicarboxylicacid)ligandsweresynthesizedasCuCl2(H2L)(4)，[Ni(HL)2】4CH3CH20H(5)，【Cu(H2L)(dipie)]‘05Glycol。2H20(6)and[Ni(H2L)(dipic)]05Glycol2H20(7)T

8、hecomplexes12and47weresynthesizedfirstlyThestructureofthesecomplexeswcrccharacterizedbysinglecrystalXraydiffraction，elementalanalysis，IRspectroscopyandUVspectroscopyInaddition，thecomplexes37werealsocharacterizedbypowderX

9、—raydiffractionThecomplexes12werecharacterizedbythermalgravimetricanalysis(TG)Mostimportantly，thecatalyticpropertiesofcomplexe817werestudiedindetailToseektheactivecatalystsforCyoxidation，a11complexeswereappliedforhomogen

10、eousoxidationwithH202asoxidantandtheeffectsofvariousfactorssuchasamountofacidandH202，temperatures，aswellasthekindofsolventwereevaluatedInaddition，theinfluenceofintermediatespeciescyclohexylhydroperoxideOntheturnovernumbe

11、rofC6H100andC6H110HwerestudiedAlso，themosteffectiveacidadditiveswerediscussedKeyWords：TransitionMetalSupramolecularComplexes；26bis(5一methyl一1H—pyrazol3一y1)pyridine；CyclohexancOxidation；HomogeneousCatalysis；Catalyticmecha