7772854Steam reforming methods and catalysts.docx
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7772854Steam reforming methods and catalysts.docx
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7772854Steamreformingmethodsandcatalysts
(37of2746)
UnitedStatesPatent
7,722,854
Watson, etal.
May25,2010
Steamreformingmethodsandcatalysts
Abstract
Thepresentinventionprovidescatalysts,reactors,andmethodsofsteamreformingoveracatalyst.Surprisinglysuperiorresultsandpropertiesobtainedinmethodsandcatalystsofthepresentinventionarealsodescribed.Forexample,acoatedcatalystwasdemonstratedtobehighlystableundersteamreformingconditions(hightemperatureandhighpressureofsteam).Methodsofmakingsteamreformingcatalystsarealsodescribed.
Inventors:
Watson;JunkoM.(Columbus,OH),Daly;FrancisP.(Delaware,OH),Wang;Yong(Richland,WA),Tonkovich;AnnaLee(Marysville,OH),Fitzgerald;SeanP.(Columbus,OH),Perry;StevenT.(Galloway,OH),Silva;LauraJ.(Dublin,OH),Taha;Rachid(Dublin,OH),AcevesdeAlba;Enrique(Dublin,OH),Chin;Ya-Huei(Richland,WA),Rozmiarek;Robert(Richland,WA),Li;XiaoHong(Richland,WA)
Assignee:
Velocy's(PlainCity,OH)
Appl.No.:
10/778,904
Filed:
February13,2004
RelatedU.S.PatentDocuments
ApplicationNumber
FilingDate
PatentNumber
IssueDate
60482351
Jun.,2003
CurrentU.S.Class:
423/652;423/418.2;423/437.1;423/653;423/654
CurrentInternationalClass:
C01B3/26 (20060101)
FieldofSearch:
423/654,653,652,418.2,437.1
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PrimaryExaminer:
Langel;Wayne
AssistantExaminer:
Fiorito;James
Attorney,AgentorFirm:
Rosenberg;Frank
ParentCaseText
RELATEDAPPLICATIONS
Inaccordancewith35U.S.C.sect.119(e),thisapplicationclaimsprioritytoU.S.ProvisionalApplicationNos.60/482,351,filedJun.25,2003.
Claims
Weclaim:
1.Amethodofmethanesteamreforming,comprising:
conductingareactioninwhichmethaneandsteamcontactacatalystatatemperatureofatleast800.degree.C.foratleast2000hourswithoutregeneratingthecatalyst;whereinthecatalystcomprisesastabilizedaluminasupportandacatalyticallyactivematerial;andwhereinthemethodisfurthercharacterizedbyacontacttimeof5msorlesswhiletheconversionofmethaneisatleast85%oftheequilibriumconversion,andwheretheconversionhasdiminishedbylessthan3%overthe2000hourswithoutregeneratingthecatalyst;andfurtherwhereinNisgreaterthan1.0;whereinNisthegrammolesofmethanefedperminutepergramofcatalyticallyactivematerial.
2.Themethodofclaim1whereinthetemperatureduringtheatleast2000hours,thetemperatureisatleast850.degree.C.andthepartialpressureofH.sub.2Oisatleast5atm.
3.Themethodofclaim2whereinthesteamtocarbonratiois3orless.
4.Themethodofclaim2whereinaveragedovertheatleast2000hoursthemethodhasa.DELTA.T.sub.approachintherange1.degree.C..times.N<.DELTA.T.sub.approach<25.degree.C..times.Nwherein.DELTA.T.sub.approachisthedifferencebetweenthepeakcatalystbedtemperatureandtheapparentequilibriumconversiontemperature;whereinthepeakcatalystbedtemperatureisthehighesttemperatureinthecatalyst.
5.Themethodofclaim4whereinastreamcontainingthemethaneandsteamispassedintoareactionmicrochannelcontainingthecatalyst.
6.Themethodofclaim1whereinthecatalysttemperatureis1000.degree.C.orless.
7.Themethodofclaim4wherein,averagedovertheatleast2000hoursthemethodhasa.DELTA.T.sub.approachintherange1.5.degree.C..times.N<.DELTA.T.sub.approach<15.degree.C..times.N.
8.Themethodofclaim3whereinheatistransferredintothecatalystfromamicrochannelheatexchangerthatisadjacenttothereactionmicrochannel.
9.Amethodofmethanesteamreforming,comprising:
passingastreamcomprisingmethaneandwaterinasteamtocarbonratioof3orless,contactingsaidstreamwithacatalystatacontacttimeof5msorlessandmaintainingthesameconditionsforatleast1000hours,whereinthereisacontinuousperiodofatleast595hoursinwhichthemethaneconversionchangesby3%orless;whereintheconversionofmethaneisatleast85%oftheequilibriumconversion;andwhereinatleast2molofmethaneareconvertedpergramcatalytically-activematerialeachminute.
10.Themethodofclaim9whereinthecatalystcomprisesRhandatleast2molofmethaneareconvertedpergramRheachminute.
11.Themethodofclaim9whereinthestreamispassedintoareactionmicrochannelcontainingthecatalyst.
12.Themethodofclaim11whereinheatistransferredintothecatalystfromamicrochannelheatexchangerthatisadjacenttothereactionmicrochannel.
13.Themethodofclaim10wherein1.degree.C..times.N<.DELTA.T.sub.approach<25.degree.C..times.Novertheatleast595hours,andtheconversionofmethaneisatleast90%oftheequilibriumconversion;whereinNisthegrammolesofmethanefedperminutepergramofcatalyticallyactivematerial;andwherein.DELTA.T.sub.approachisthedifferencebetweenthepeakcatalystbedtemperatureandtheapparentequilibriumconversiontemperature;whereinthepeakcatalystbedtemperatureisthehighesttemperatureinthecatalyst.
14.Themethodofclaim10wherein1.degree.C..times.N<.DELTA.T.sub.approach<5.degree.C..times.Novertheatleast595hours;whereinNisthegrammolesofmethanefedperminutepergramofcatalyticallyactivematerial;andwherein.DELTA.T.sub.approachisthedifferencebetweenthepeakcatalystbedtemperatureandtheapparentequilibriumconversiontemperature;whereinthepeakcatalystbedtemperatureisthehighesttemperatureinthecatalyst.
15.Themethodofclaim5wherein1.degree.C..times.N<.DELTA.T.sub.approach<5.degree.C..times.Novertheatleast2000hours;whereinNisthegrammolesofmethanefedperminutepergramofcatalyticallyactivematerial;andwherein.DELTA..sub.approachisthedifferencebetweenthepeakcatalystbedtemperatureandtheapparentequilibriumconversiontemperature;whereinthepeakcatalystbedtemperatureisthehighesttemperatureinthecatalyst.
16.Themethodofclaim2whereinthecatalystcomprisesRhandatleast2molofmethaneareconvertedpergramRheachminute.
17.Themethodofclaim1whereinthemethaneandsteamflowintocontactwiththecatalystinasteamtocarbonratioof3:
1to1:
1.
18.Themethodofclaim17whereinthestabilizedaluminasupportisstabilizedwithMg.
19.Amethodofmethanesteamreforming,comprising:
conductingareactioninwhichmethaneandsteamcontactacatalystatatemperatureofatleast800.degree.C.foratleast1000hourswithoutregeneratingthecatalyst;whereinthecatalystcomprisesastabilizedaluminasupportandacatalyticallyactivematerial;andwhereinthemethodisfurthercharacterizedbyacontacttimeof5msorlesswhileachievinganaverageapproachtoequilibriumconversionofgreaterthan90%andfurtherwhereintheconversionhasdiminishedbylessthan3%overthe1000hourswithoutregeneratingthecatalyst;andfurtherwhereinNisgreaterthan1.0;whereintheaverageapproachtoequilibriumconversionistheratioofmeasurablehydrocarbonconversiontoequilibriumhydrocarbonconversion;whereinNisthegrammolesofmethanefedperminutepergramofcatalyticallyactivematerial.
20.Themethodofclaim19whereinthecatalystcomprisesRh.
21.Themethodofclaim18whereinthecatalystcomprises1to3wt%Rh.
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