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1、pubs.acs.org/Langmuir©2010AmericanChemicalSocietyDirectSynthesisofHydrogenPeroxideandBenzylAlcoholOxidationUsing†Au-PdCatalystsPreparedbySolImmobilization†††‡‡JamesPritchard,LokeshKesavan,MarcoPiccinini,QianHe,RamchandraTiruvalam,††††NikolaosDimitratos,Jos
2、eA.Lopez-Sanchez,AlbertF.Carley,JenniferK.Edwards,‡,†ChristopherJ.Kiely,andGrahamJ.Hutchings*†SchoolofChemistry,CardiffUniversity,MainBuilding,ParkPlace,CardiffCF103AT,UnitedKingdom,and‡CenterforAdvancedMaterialsandNanotechnology,LehighUniversity,5EastPack
3、erAvenue,Bethlehem,Pennsylvania18015-3195ReceivedApril21,2010.RevisedManuscriptReceivedApril28,2010WereportthepreparationofAu-Pdnanocrystallinecatalystssupportedonactivatedcarbonpreparedviaasol-immobilizationtechniqueandexploretheiruseforthedirectsynthesis
4、ofhydrogenperoxideandtheoxidationofbenzylalcohol.Inparticular,weexaminethesynthesisofasystematicsetofAu-PdcolloidalnanoparticleshavingarangeofAu/Pdratios.ThecatalystshavebeenstructurallycharacterizedusingacombinationofUV-visiblespectroscopy,transmissionele
5、ctronmicroscopy,STEMHAADF/XEDS,andX-rayphotoelectronspectroscopy.TheAu-Pdnanoparticlesarefoundinthemajorityofcasestobehomogeneousalloys,althoughsomevariationisobservedintheAuPdcompositionathighPd/Auratios.Theoptimumperformanceforthesynthesisofhydrogenperox
6、ideisobservedforacatalysthavingaAu/Pd1:2molarratio.However,thecompetinghydrogenationreactionofhydrogenperoxideincreaseswithincreasingPdcontent,althoughPdaloneislesseffectivethanwhenAuisalsopresent.Investigationoftheoxidationofbenzylalcoholusingthesemateria
7、lsalsoshowsthattheoptimumselectiveoxidationtothealdehydeoccursfortheAu/Pd1:2molarratiocatalyst.ThesemeasuredactivitytrendsarediscussedintermsofthestructureandcompositionofthesupportedAu-Pdnanoparticles.Introductionparticularlyeffectiveforthedirectsynthesis
8、ofhydrogenperoxide14,1516fromitselementsandtheoxidationofalcohols.InthisSupportedmetalnanoparticlesarereceivingsignificantatten-paper,weexaminesupportedAu-Pdalloynanoparticlespreparedtionascatalystsforabroadr