Evolution of Gold Species in an Au/CeO2 Catalyst and Its Impact on Activity for CO Oxidation

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摘要 AnAu/ceria(0.44%,massfraction)catalystcontaininggoldionswaspreparedbyamodifieddepositionprecipitationmethod,andtheevolutionofgoldionsinthecatalystanditsinfluenceonthecatalysisofCOoxidationwereinvestigated.Itwasfoundthattheas-preparedcatalystcontaininggoldionswithhighvalencecouldfullyoxidizeCOat–10°CinitiallybutwasdeactivatedgraduallyatlowtemperaturesduringthereactionwithCOortreatmentbyunpurifiedair.ThedeactivationofthecatalystduringCOoxidationortreatmentofitbyunpurifiedairwasindependentandprogressiveatlowtemperatureswhiletheactivityofthecatalystatrelativelyhightemperatureswasmaintainedwell.DuringthereactionwithCOortreatmentbyunpurifiedair,theXPSresultsindicatethatgoldspeciesevolvedfromhighvalencetolowvalenceandthediffusereflectanceUV-Visspectrashowthathighvalencegoldwasreducedtochargedgoldclusters,goldclustersgrewtosmallgoldcrystalsandsmallgoldcrystalsgrewtolargegoldparticles.Accordingly,thehighvalencegoldcorrespondedtotheactivityatlowtemperaturesandthemetallicgoldwasactiveandrelativelystableathightemperatures.Theturnoverfrequencies(TOF)ofthecatalyststreatedbydifferentmethodsat273Kdecreasedwiththeevolutionofgoldspeciesfromhighvalencetolowvalence,nomaximumofTOFwasobservedalthoughgoldparticlesinthecatalystattainedtoabout2―3nmduringthetreatment.AnAu/ceriacatalystwithagoldloadof0.87%(massfraction)maintainedagoodactivityforCOoxidationwithin18hatroomtemperature.Thecatalystswerecharacterizedviatransmittedelectronicmicroscopy(TEM),inductivelycoupledplasmaopticalemissionspectrometry(ICP-OES),X-raydiffraction(XRD)andBETspecificsurfaceareaandUV-VisDRSaswell.
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出版日期 2010年03月13日(中国期刊网平台首次上网日期,不代表论文的发表时间)
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