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1、KineticsandCatalysisoftheWater-Gas-ShiftReaction:AMicrokineticandGraphTheoreticApproachADissertationSubmittedtotheFacultyoftheWORCESTERPOLYTECHNICINSTITUTEDepartmentofChemicalEngineeringInpartialfulfillmentoftherequirementsfortheDegreeofDoctorofPhilosophyinChemicalEngineeringby____________
2、__________________________CaitlinA.CallaghanMarch31,2006________________________________________________________________________________ProfessorRavindraDatta,AdvisorProfessorIlieFishtik,Co-AdvisorWPIChemicalEngineeringDepartmentWPIChemicalEngineeringDepartment_____________________________
3、___________________________________________________ProfessorNikolaosK.KazantzisProfessorJosephD.FehribachWPIChemicalEngineeringDepartmentWPIMathematicalSciences&ChemicalEngineeringDepartment________________________________________________________________________________ProfessorJenniferL.W
4、ilcoxDr.A.AlanBurkeWPIChemicalEngineeringDepartmentNavalUnderseaWarfareCenter,Newport,RI________________________________________ProfessorDavidDiBiasio,Dept.HeadWPIChemicalEngineeringDepartmentABSTRACTThesearchforenvironmentallybenignenergysourcesisbecomingincreasinglyurgent.Onesuchtechnolo
5、gyisfuelcells,e.g.,thepolymerelectrolytemembrane(PEM)fuelcellwhichuseshydrogenasafuelandemitsonlyH2O.However,reforminghydrocarbonfuelstoproducetheneededhydrogenyieldsreformatestreamscontainingCO2aswellasCO,whichistoxictothePEMfuelcellatconcentrationsabove100ppm.AstheamountofCOpermittedtore
6、achthefuelcellincreases,theperformanceofthePEMfuelcelldecreasesuntilitultimatelystopsfunctioning.Thewater-gas-shift(WGS)reaction,CO+H2ODH2+CO2,providesamethodforextractingtheenergyfromthetoxicCObyconvertingitintousableH2alongwithCO2whichcanbetoleratedbythefuelcell.Althoughawellestablishedi
7、ndustrialprocess,alternatecatalystsaresoughtforfuelcellapplication.CatalystselectionfortheWGSreactionhas,untilrecently,beenbasedontrial-and-errorscreeningofpotentialcatalystsduetoalackoffundamentalunderstandingofthecatalyst’sfunctioning.Forthisreason,weembarke
