Au Promotional Effects on the Synthesis of H2O2 Directly from H2 and O2 on Supported

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1、84102007,111,8410-8413PublishedonWeb05/26/2007AuPromotionalEffectsontheSynthesisofH2O2DirectlyfromH2andO2onSupportedPd-AuAlloyCatalystsYi-FanHan,*,²ZiyiZhong,²KanaparthiRamesh,²FengxiChen,²LuweiChen,²TimWhite,³QiulingTay,³SitiNurbayaYaakub,²andZhanWang²InstituteofChemicalandEngineeringSc

2、iences,1,PesekRoad,JurongIsland,Singapore627833,andSchoolofMaterialsScienceandEngineering,NanyangTechnologicalUniVersity,50NanyangAVenue,Singapore639798ReceiVed:April16,2007;InFinalForm:May17,2007SupportedPd,Au,andPd-AualloycatalystsarecharacterizedwithinsitudiffusereflectanceinfraredFou

3、riertransformspectroscopyofCOadsorption(DRIFTS),quantitativepowderX-raydiffraction,andX-rayphotoelectronspectroscopy.ThespectroscopicresultspresentedinthepaperdemonstratetheexistenceofelectrondensitytransferbetweenPdandAuatomsinalloysurfaces.Inparticular,themodificationofthePdelectronics

4、tructurebytheadditionofAuisconfirmedprobablyforthefirsttimebytheDRIFTspectra.Therelationshipbetweensurfacecompositionandcatalystperformanceinthesynthesisofhydrogenperoxidedirectlyfromhydrogenandoxygenwasestablished.PreliminaryresultsindicatethattheactivityandselectivityofPd-Aualloycataly

5、stscanbesignificantlyenhancedthroughadjustingthesurfacestructuresbychangingtheAucontentinalloys.1.Introductiontodevelopaneffectivecatalyticsystemthatcanenhancetheyieldandselectivitysimultaneously.4SignificantimprovementsNanosizedpalladium-goldcrystalsareusedtocatalyzeahavebeenachievedbyu

6、singPdorPd-alloyedcatalystswithnumberofreactionssuchasCOoxidation,thesynthesisofvinylsecondarymetalssuchasAuandPtcatalysts.5Amongthem,acetatemonomerandhydrogenperoxide(H2O2),hydridethePd-Aualloyhasproventobeapromisingcatalyst;forchlorinationofCCl2F2,hydrogenationofhydrocarbons,cyclo-exam

7、ple,Hutchingsandco-workersobservedanimprovedtrimerizationofacetylene,andtheoxidationofprimaryalcoholscatalyticperformanceforthisreactiononPd-Aucatalyststoaldehydes.1ThepromotionaleffectofAuintheAu-PdalloysupportedonTiO2,Fe2O3,andZrO2inabatchreactorat2°Ccatalystshasbeenthe