•  
  •  
 

Corresponding Author

Bing-liang WU

Abstract

Two local electrochemical reactive interfaces are established using two strips of Nafion~ membrane separated each other, which are in contact with different surface regions of the same metal-sheet working electrode. One potentiostatis used to control thepotentialof one electrochemical reactive interface to generate adsorbed surface speciesand the other potentiostatto hold the potential of the second interface as a detector of the intermediate. The adsorbed surface species driven by the difference in surface concentration diffuses alongthe surface of the metal-sheet between both local electrochemical interfaces and can be detected at the second interface when they achieveover there.The surface diffusion coefficient of the oxygen-containing surface species on Pt was measured, then the synergisticcatalysis was studied using a simplified model Pt-Ru electrode and the spillover of OH_(ads)from the surface of Pt to the surface of Ru was not found in the experimental potential region. This would be explained asthat the realization of synergistic effect is due to spillover of the toxic adsorbed intermediate CO_(ads)on Pt to the surface of Ru and CO_(ads) is oxidized into CO_(2 )by the oxygen-containing surface species over there.

Keywords

Adsorbed intermediate, Surface diffusion, Spillover, Pt-Ru electrode, Electrocatalysis

Publication Date

2004-08-28

Online Available Date

2004-08-28

Revised Date

2004-08-28

Received Date

2004-08-28

References

[1] KapoorA,YangRT,WongC.Surfacediffusion[J].Catal.Rev.,1989,31:129.
[2] ConnerWC,FalconerJL.Spilloverinheterogeneouscatalysis[J].Chem.Rev.,1995,95:759.
[3] TuWY,LiuWJ,ChaCS,etal.Studyofthepowder/membraneinterfacebyusinthemicroelectrodetechniqueI.ThePt black/Nafioninterface[J].ElectrochimicaActa,1998,43:3731.
[4] PaulusUA,VeziridisZ.SchnyderB,etal.Fundamentalinvestigationofcatalysisutilizationattheelectrode/solidpolymerelectolyetinterface.PartI.Developmentofamodelsystem[J].J.ElectroanalyticalChemistry,2003,541:77.
[5] LiuWJ,WuBL,ChaCS.DeterminationofsurfacediffusioncoefficientsofhydrogenadatomandsurfaceOHradicalonplatinumelectrode[J].J.Russ.ofElectrochem.,2002,36:846.
[6] TienTTsong.AhistoricperspectiveofFIMandSTMstudiesofsurfacediffusion[J].MaterialsScienceandEngineeringA,353(2003)1.
[7] MakCH,BrandJL,DeckertAA.SurfacediffusionofhydrogenonRu(001)studiedusinglaser inducedthermaldesorption[J].Chem.Phys.,1986,85:1676.
[8] CandauJFC,ConnerWC.Thespilloverofhydrogenontosilican[J].J.Catalysis,1987,106:378.
[9] AngersteinKozlowskaH,ConwayBE,SharpWBA.Therealconditionofelectrochemicallyoxidizedplatinumsurface.PartI.Resolutionofcomponentprocesses[J].J.Electroanal.Chem.,1973,43:9.
[10] FrelinkT,VisscherW,CoxAP.EllipsometryandDEMSstudyoftheelectrooxidationofmethanolatPtandRuandSn promotedPt[J].Electrochim.Acta,1995,40:1537.
[11] HideakiKita,ShenYe,YunzhiGao.MasstransfereffectinhydrogenevolutionreactiononPtsinglecrystalinacidsolution[J].J.Electroanal.Chem.,1992,334:351.
[12] KwasniewskiVJ,SchmidtLD.SurfacediffusionofcarbonmonoxideonPt(111)[J].SurfaceScience,1992,274:329.
[13] DayJB,VuissozPA,OldfieldE,etal.Nuclearmagneticresonancespectroscopestudyoftheelectrochemicaloxidationproductofmethanolonplatinum[J].J.Amer.Chem.Soc.,1996,118:13046.
[14] HubertAGasteiger,NenadMarkovic,PhilipNRoss,etal.COelectrooxidationonwell characterizedPt Rualloys[J].J.Phys.Chem.,1994,98:617.

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.