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IntroductionThedesignandsynthesisofnoveltransition-metal-substitutedpolyoxometalate(TMSP)clustersbasedontheclassicallacunaryKegginorDawsonfragmentshaveraisedextremeinterestduetotheirstructuralvarietiesandunexpectedproperties,whichgivesrisetopotentialapplicationsinmagnetism,materialsciences,catalysis,andbiomedicine..Threenovelhexa-Ni-substitutedDawsonphosphortungstateshavebeenmadeunderhydrothermalconditionsandwerecharacterizedbyIRspectroscopy,elementalanalysis,diffusereflectancespectroscopy,thermogravimetricanalysis,powderX-raydiffraction,andsingle-crystalX-raydiffraction.(1)[Ni6(en)3(H2O)6(OH)3(H3P2W15O56)]·14H2O(2)[Ni(enMe)2(H2O)][Ni6(enMe)3(OH)3(H2O)6(HP2W15O56)]·10H2O(3)[Ni(enMe)2]3[Ni(enMe)2(H2O)][Ni(enMe)(H2O)2][Ni6(enMe)3(OH)3(Ac)2(H2O)(P2W15O56)]2·6H2OHydrothermalCombinationofTrilacunaryDawsonPhosphotungstatesandHexanickelClusters:FromanIsolatedClustertoa3DFrameworkXin-XiongLi,[a]Wei-HuiFang,[a]Jun-WeiZhao,*[b]andGuo-YuYang*[a,c]FujianInstituteofResearchontheStructureofMatterChem.Eur.J.2014,20,1–10Synthesisofcompound2,31Synthesisofcompound1Structureofcompound1,2figure1:en=ethylenediamine,enMe=1,2-diaminopropane,Ac=CHCOO-Colorcodes:WO6:red,PO4:yellow,NiO6/NiO2N2(H2O)2:greenfigure1figure2figure2:a)ViewofthestackingfashionofDawsonpolyanionsin1alongtheaaxis;b)ViewofthestackingfashionofDawsonpolyanionsin2alongthecaxis.Structureofcompound3figure3:Theneighboringchainswereinterlinkedby[Ni(enMe)2]2+bridgestofroma2Dlayer(d)Colorcodes:WO6=red,NiO6andNiO4N2:green,PO4=yellowfigure3figure4Figure4:Temperaturedependenceofthemolarmagneticsusceptibilityandtheproductofthemolarmagneticsusceptibilityandthetemperatureforcompound3between2.0and300K.TGcurveForcompounds1–3,thegoodaccordancebetweentheexperimentalandsimulatedpowderXRDpatternsindicatesthegoodphasepurityofthesamples.ConclusionThisstudyprovidesnotonlyavaluablemolecularmodelofthe“Co−Pi”catalystswithawell-definedstructurebutalsoanunprecedentedopportunitytofine-tunehigh-nuclearityPOMclustersforvisiblelight-drivenwatersplitting.Theirphotocatalyticwateroxidationactivitieshavebeensystematicallyinvestigatedandshowedthat1−4arealleffectivemolecularcatalystsandthephotocatalyticperformanceis3≤142undervisiblelightirradiation.As1−4areaseriesofSi-centered,Ge-centered,P-centered,andAs-centeredPOMswithanalogousstructure,thecomparisonofthecatalyticactivityamong1−4forwateroxidationprovidesvaluableinsightintotheinfluenceofheteroatomsonoxygenevolutionaswellasthefurtherdesignandsynthesisofmorestableandefficientWOCs.Multipleexperimentscollectivelyconfirmedthatcompounds1−4aregenuinemolecularcatalystsandmaintaintheirstructuralintegrityunderthephotocatalyticconditions.
本文标题:海报(poster)模板(英文)
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