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1、Letterpubs.acs.org/JPCLGasificationMechanismofCarbonwithSupercriticalWateratVeryHighPressures:EffectsonH2Production†,†††NicolasMartin-Sanchez,FranciscoSalvador,*M.JesusSanchez-Montero,andCarmenIzquierdo†DepartamentoQuímicaFísica,FacultaddeCienciasQuími
2、cas,UniversidaddeSalamanca,PlazadelaMerceds/n37008Salamanca,Spain*SSupportingInformationABSTRACT:Thescarcedataconcerningthegasificationofcarbonaceoussolidswithsupercriticalwater(SCW)suggestthegreatpotentialofthismethodtoproduceavaluablegreenfuelsuchas
3、H2.However,theextraordinarypropertiesofSCWhavenotbeenproperlyappliedtoH2productionbecausethemechanismthatgovernsgasificationundertheseconditionsremainsunclear.Here,wepresentastudyinwhichthisreactionisexploredwithinthelargestpressurerangeeverassayedint
4、hisfield,from1to1000bar.TheamplitudeoftheexperimentalconditionsinvestigatedhighlightsthevariouspathwaysthatgoverngasificationwithsteamandSCW.Undersupercriticalconditions,theclustersformedaroundthesuperficialgroupsofthesolidreducetheenergeticrequirements
5、forgasificationandgenerateCO2asaprimaryproductofthereaction.Consequently,gasificationwithSCWissignificantlyfasterthanthatusingsteam,andtheproducedgasesarericherandmoreappropriatetoobtainpureH2.SECTION:Surfaces,Interfaces,PorousMaterials,andCatalysisThep
6、ropertiesofH2makeitagreenfuelwiththepotentialrateofgasificationwithsteamiscontrolledbytheslowtobeusedasanenergycarrier.However,itsproductiondesorptionofCOfromtheoxygenatedgroupsC(O)(stage6−8mustbeoptimizedtoconstituteacompetitivealternative3).againsto
7、therenergysources.ThegasificationofcarbonaceousOthersecondaryreactionsoccurduetothecharacteristicsolidswithhigh-temperaturesteamistheoldestmethodforwaterexcessofthesesystems.Accordingtothewater−gasshiftobtainingH2,althoughcurrentlymostH2producedcomesr
8、eaction,stage4,otherwatermoleculesareabletoconvertafromCH4steamreforming.ThegasificationprocedureportionofthedesorbedCOintoCO2andmoreH2,althoughgeneratesasyntheticgasprincipallyformedbyH2,CO,andCO2maybealsogeneratedbytheinverseoftheBoudouardCO2.Itcons
