Chemical-Looping Combustion of Simulated Synthesis Gas Using_中华文本库
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1584Energy&Fuels,Vol.21,No.3,2007
CLCtestwasconductedatdifferenttemperaturesat100psiusingthefollowingmixedgases:12%CO2,36%CO,25%He,and27%H2forreductionandairforoxidation.Toavoidthemixingofreductiongasmixtureandair,thesystemwasflushedwithargonfor5minbeforeandaftereachreactionphase.LABTECHNOTEBOOKprowasusedtomonitorthereactorpressureduringtheexperiments.
TaperedElementOscillatingMicrobalance(TEOM).Thetaperedelementoscillatingmicrobalance(TEOM)Series1500pulsemassanalyzer(PMA1500fromRupprecht&PatashnickCo.Inc.,Albany,NY)wasusedtostudytheeffectofpressureontherateofuptakeofNiO/bentonite.Thissystemconsistsofamicroreactorwithahigh-resolutionmicrobalancethatgeneratesreal-timemeasurementsofmasschangesduringgas-solidreactions.17Itincludesataperedelementoscillatingmicrobalance(TEOM)consistingofatubeinwhichthesamplebedcanbepackedatitslowerendbetweenquartzwool.InsidetheTEOM,therearetwotemperature-controlledzones.Thepreheatzonecontrolstheinletgasstreamtemperatureofthetaperedelementandthesamplebed.17,18TheTEOMperformanceisquantifiedintermsofthenormalizedstandarddeviation(NSD).TheNSDisanindicatorofanynoiseinthetestbedanddependsuponhowwellthesampleispackedandwhetherthereisothermechanicalorelectricaldisturbance.17,18IntheTEOM,thesteadyflowofgasthroughthesampleprovidescompletecontactwiththesamplebed.ThereactiongaswasintroducedtoNiO/bentoniteoxygencarrierbed(particlesize:30mesh)ataflowrateof45cm3/min.Thereactiongasutilizedforreductionconsistedof12%CO2,36%CO,25%He,and27%H2,andairwasutilizedfortheoxidation.Thereductionreactiontimewas10min,andtheoxidationreactiontimewas60minforallexperiments.Toavoidthemixingofreductiongasmixtureandair,thesystemwasflushedwithargonfor5minbeforeandaftereachreactionphase.One-cycletestswereconductedat800°Candatpressuresof1atmand50and100psi.AllconditionsandflowrateswerecontrolledwithsoftwarecreatedinLabView,whichwascommerciallymadeavailablethroughRupprecht&PatashnickCo.Inc.
3.CharacterizationofOxygenCarrierParticles.X-raydiffractionandX-rayphotoelectronspectraoftheoxygencarrierparticlesreactedinthehigh-pressureflowreactorwerestudiedtodetermineiftherewasphasetransformationandchangesinthemorphologyintheNiObentoniteoxygencarrierparticleduringmulticyclechemical-loopingcombustion.X-raydiffractionofunreactedNiObentoniteoxygencarrierandthosereactedinthehighpressurepackedbedreactorwascarriedoutusingaPanAnalyticalX’PertProX-raydiffractorutilizingCuKRradiation.Thediffractionpatternswereobtainedbetween2θ)10°and80°.DataanalysiswasconductedwithHighScorePlusanalysissoftwaresuppliedbyPanAnalytical.X-rayphotoelectronspectra(XPS)wererecordedonaPhysicalElectronics(PHI)SAM-590ultrahighvacuum(UHV)systemequippedwithaPHI50-096X-rayphotoelectronspectroscopysubsystem,aPHIsphericalcapacitortypeanalyzerwithanOmniFocusIIIlens,andaPHI04-548duelanodeX-raysource.SystemcalibrationwasinaccordancewithPHIproceduresutilizingthephotoemissionlinesEB(Cu2p3/2))932.7eV,EB(Au4f7/2))84eV,andEB(Ag3d5/2))368.3.19Thesystemhadastandingpressureof10-9Torr(1.3×10-7Pa)andwas-7operatedwithinapressurerangeof10-9-10-8Torr(1.3×10to1.3×10-6Pa).Thebindingenergieswerecorrectedutilizingthereferencebindingenergyforadventitiouscarbon,C(1s1/2))284.8eV.Allreportedintensitieswereexperimentallydeterminedaspeakareasdividedbytheinstrumentalsensitivityfactors.DataanalysiswasconductedwithMultipakanalysissoftwaresuppliedbyPhysicalElectronics.Surfacemorphologyand
(17)Patachnick,H.:Rupprecht,G.:Wang,J.C.F.ACSSymp.Ser.-193.
(18)Jalani,N.H.;Datta,R.J.Membr.Sci.-2),167-175.(19)Moulder,J.F.;Stickle,W.F.;Sobol,P.E.;Bomben,K.D.HandbookofX-RayandultraVioletPhotoelectronSChastain,J.;King,R.C.,Jr.Eds.;PhysicalElectronicsInc.:EdenPrarie,MN,1992,
Siriwardaneetal.
Figure1.Ten-cyclethermogravimetricanalysisofNiO/bentonite(200mesh)withcoal-derivedsynthesisgasatatemperatureof800°C.
<positionoftheSimulatedSynthesisGasUsedfor
componentmole%COH38CH230.8H4CO2O16.50.N0.12182
qualitativecompositionoftheoxygencarrierparticlesusedinmulticycleTGAtestsweredeterminedutilizingaJEOL-6300scanningelectronmicroscope(JEOL-6300FESEM).TheJEOL-6300isequippedwithanET-typesecondaryelectrondetectorandanUltra-DrySiliconDriftdetectorinterfacedtoaThermo-NoranSystemSixmicroanalysissystem.The-instrument7-10-6wasroutinelyoperatedwithinapressurerangeof10Torr(1.3×10-5to1.3×10-4Pa).Themicroanalysissystem,priortoanalysis,wascalibratedusingaCustandard,withthecentroidoftheKRspectralpeak(s)beingreferencedtotheenergyvalueof8.046keV.SurfaceareameasurementofbentonitepowderandNiO/bentonitewascarriedoutusingavolumetricgassorptionapparatusautosorb-6,Quantachrome.
ResultsandDiscussion
ThecompositionofthesimulatedsynthesisgasusedforreductioninatypicalgasificationsystemisgiveninTable1.Chemicalequationsforoxidationwithoxygenandreductionreactionwiththeabovegascompositioncanbepresentedasfollows.Reduction
0.55206CO+0..+NiOf
0.+0.44843H2O+Ni;
?H)-20.52MJ/kmol(3)Oxidation
Ni+0.5O2fNiO;?H)-244.30MJ/kmol(4)
Bothreactionsareexothermic.
Ifthefuelwiththeabovegascompositioniscombustedinaconventionalreactor,thechemicalequationcouldberepresentedas
0.55206CO+0..+0.5O2f
0.+0.44843H2O;
?H)-264.9905MJ/kmole(5)TheheatevolvedduringCLC(eq1and2)andthatfromtheconventionalreactor(eq5)isnearlysame.
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solid-state physical electronics
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