新型铁ⅱ 钴ⅱ配合物的合成及其催化乙烯齐聚行为的分析-synthesis of a new iron ⅱ cobalt ⅱ complex and analysis of its catalytic behavior for ethylene oligomerization.docxVIP

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新型铁ⅱ 钴ⅱ配合物的合成及其催化乙烯齐聚行为的分析-synthesis of a new iron ⅱ cobalt ⅱ complex and analysis of its catalytic behavior for ethylene oligomerization.docx

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新型铁ⅱ 钴ⅱ配合物的合成及其催化乙烯齐聚行为的分析-synthesis of a new iron ⅱ cobalt ⅱ complex and analysis of its catalytic behavior for ethylene oligomerization

AbstractLatetransitionmetalcomplexisakindofcatalystwithstableperformanceandhighcatalyticactivity.Thenon-metalloceneolefinpolymerizationcatalysthasarousedgreatattentioninacademicandindustrialresearchduringthepasttwodecades.Designingselectivelycatalyticmetalcomplexeshavegreatpracticalvalueinethyleneoligomerization.Inthispaper,aseriesofiron,cobaltcomplexescontainingN~N~Ntridentateligandswassynthesizedtoexploretheircatalyticbehaviorinethyleneoligomerization.Allthecomplexesshowedhighethylenedimerizationselectivity.Thisthesisisdividedintothreeparts:2-(1-methyl-2-benzimidazolyl)-6-acetylpyridineandsixdifferentanilinessubstitutedbybenzhydrylwerefirstlysynthesized.Withacatalyticamountofp-toluenesulfonicacid,aseriesof2-(1-methyl-2-benzimidazolyl)-6-(1-(arylimino)ethyl)pyridineN~N~Ntridentateligandswassynthesizedbycondensation.Allorganiccompoundswerefullycharacterizedby1HNMR,13CNMR,IR,elementalanalysis.Thecorrespondingcobalt(Ⅱ)andiron(Ⅱ)2-(1-methyl-2-benzimidazolyl)-6-(1-(arylimino)ethyl)pyridylcomplexesweresynthesizedbycoordinationwithCoCl26H2OandFeCl2?4H2O.IncomparisonwiththeIRspectraoftheligands,theC=Nstretchingvibrationsincomplexeswereshiftedtowardlowerfrequencies,whichindicatedaneffectivecoordinationinteractionbetweentheiminonitrogenatomandtheiron/cobaltcenter.TheX-raycrystallographicstudiesonthetridentateCo3complexerevealedthecoordinationgeometryasadistortedtrigonalbipyramid.Thefive-coordinatestructurewasformedbycombinatingthecentralmetalcobalt,tridentateligandwithtwochlorineatoms.Allthestructureofthecomplexeswasfurtherconfirmedbyelementalanalysis.Co6wastreatedwithmethylaluminoxane(MAO),modifiedmethylaluminoxane(MMAO)respectively.Thecomplexshowedthelowcatalyticactivityof102g(molofCo)-1h-1underdifferentreactionconditions.WhileFe6showedthemoderateIIcatalyticactivityof4.9×104g(molofFe)-1h-1whenactivatedbyMMAO.Bothofthemshowedhighselectivityof1-butene.Then,theactivityofalltheironcomplexeswereexploredunderthereactionconditionofMMAO,10atmofethylene,30oC.Fe1complexdisplayedtheh