AmericanInstituteofAeronauticsandAstronautics0924071KineticModelingoftheH2/O2ReactioninHigh-PressureFlamesMichaelP.Burke,1YiguangJu,2andFrederickL.Dryer3DepartmentofMechanicalandAerospaceEngineering,PrincetonUniversity,Princeton,NJ08544MarcosChaos4FireandExplosionsDynamicsGroup,FMGlobalEngineeringandResearch,Norwood,MA02062StephenJ.Klippenstein5ChemicalSciencesandEngineeringDivision,ArgonneNationalLaboratory,Argonne,IL60439AnupdatedH2/O2chemical-kineticmodelbasedonthatofLietal.[Int.J.Chem.Kinet.36(2004)566-575]istestedagainstawiderangeofcombustiontargetsthatincludethepreviousvalidationsetfromLietal.aswellasnewmeasurementsthathavebecomeavailableforspeciationduringH2oxidation,H2Odecomposition,andH2O2decomposition;ignitiondelaytimesinshocktubesandrapidcompressionmachines;andhigh-pressureand/orlow-flame-temperatureflamespeeds.Duringtheconstructionofthepresentmodel,wehaveattemptedtoidentifymajorsourcesofuncertaintiesinthemodelthatresultinuncertaintiesinpredictionsofrelevantcombustionbehaviorinordertofacilitatefurthermodelimprovementsinthefuture.Here,wepresentanalysesthatsuggestthatimprovedcharacterizationofbath-gasmixturebehaviorinunimoleculardecompositionreactionsislikelytobenecessarytopredictignitiondelaytimesandflamespeedsaccurately.Anumberofrateconstantexpressionsfromrecentelementaryreactionstudieshavebeenincorporated.PredictionsusingthepresentmodeladequatelyreproduceallthetargetsusedforvalidationofLietal.andyieldsignificantlyimprovedagreementwithmorerecenttargetsthatincludehigh-pressure,diluteflames.I.IntroductionheH2/O2systemisafundamentaltopicincombustionsciencethathashistoricallyreceivedsignificantattentionduetobothitsrichkineticbehavioranditsimportancetoavarietyofapplicationsinenergyconversion.SinceH2andtheintermediateoxidationspeciesarealsodominantintermediatespeciesintheoxidationofallhydrocarbonandoxygenatedfuels,theH2/O2mechanismnotonlyformsanessentialsubsetofanyhydrocarbonoroxygenateoxidationmechanism1butalsocontainsanumberofreactionsthathaverateconstants...
