简介:ThecorrelationbetweenphasestructuresandsurfaceacidityofAl2O3supportscalcinedatdifferenttemperaturesandthecatalyticperformanceofNi/Al2O3catalystsintheproductionofsyntheticnaturalgas(SNG)viaCOmethanationwassystematicallyinvestigated.Aseriesof10wt%NiO/Al2O3catalystswerepreparedbytheconventionalimpregnationmethod,andthephasestructuresandsurfaceacidityofAl2O3supportswereadjustedbycalciningthecommercialγ-Al2O3atdifferenttemperatures(600–1200C).COmethanationreactionwascarriedoutinthetemperaturerangeof300–600Catdifferentweighthourlyspacevelocities(WHSV=30000and120000mL·g-1h-1)andpressures(0.1and3.0MPa).ItwasfoundthathighcalcinationtemperaturenotonlyledtothegrowthinNiparticlesize,butalsoweakenedtheinteractionbetweenNinanoparticlesandAl2O3supportsduetotherapiddecreaseofthespecificsurfaceareaandacidityofAl2O3supports.Interestingly,NicatalystssupportedonAl2O3calcinedat1200C(Ni/Al2O3-1200)exhibitedthebestcatalyticactivityforCOmethanationunderdifferentreactionconditions.LifetimereactiontestsalsoindicatedthatNi/Al2O3-1200wasthemostactiveandstablecatalystcomparedwiththeotherthreecatalysts,whosesupportswerecalcinedatlowertemperatures(600,800and1000C).ThesefindingswouldthereforebehelpfultodevelopNi/Al2O3methanationcatalystforSNGproduction.
简介:Inthiswork,syngasmethanationoverNi-W/TiO2-SiO2catalystwasstudiedinafluidized-bedreactor(FBR)anditsperformancewascomparedwithafixed-bedreactor(FIXBR).Theeffectsofmainoperatingvariablesincludingfeedstockgasesspacevelocity,cokecontent,bedtemperatureandsulfur-tolerantstabilityof100hlifewereinvestigated.ThestructureofthecatalystswascharacterizedbyXRD,N2adsorptiondesorptionandTEM.Itisfoundthatundersamespacevelocityfrom5000h1to25000h1FBRgaveahigherCH4yield,lowercokecontent,andlowerbedtemperaturethanthoseobtainedinFIXBR.Ni-W/TiO2-SiO2catalystpossessedexcellentsulfur-tolerantstabilityonthefeedstockgaseslessthan500ppmH2SinFBR.ThecarbondepositsformedonthespentcatalystwereintheformofcarbonfibersinFBR,whileintheformofdenseaccumulationdistributionappearanceinFIXBR.
简介:HydrotalciteprecursorsofLamodifiedNi-Al2O3andNi-SiO2catalystspreparedbyco-precipitationmethodandthecatalyticactivitieswereexaminedfortheproductionofCOx-freeH2byCH4decomposition.Physico-chemicalcharacteristicsoffresh,reducedandusedcatalystswereevaluatedbyXRD,TPRandO2pulsechemisorptions,TEMandBET-SAtechniques.XRDstudiesshowedphasesduetohydrotalcite-likeprecursorsinovendriedformproduceddispersedNiOspeciesuponcalcinationinstaticairabove450C.Ramanspectraofdeactivatedsamplesrevealedthepresenceofbothorderedanddisorderedformsofcarbon.Ni-La-Al2O3catalystwithamoleratioofNi:La:Al=2:0.1:0.9exhibitedtremendouslyhighlongevitywithahydrogenproductionrateof1300molH2mol1Ni.AdirectrelationshipbetweenNimetalsurfaceareaandhydrogenyieldswasestablished.
简介:测量了ZnO-TiO2-Bi2O3-CuO-Co2O3,ZnO-TiO2-Bi2O3-CuO-Cr2O3,ZnO-TiO2-Bi2O3-CuO-MnO2和ZnOTiO2-Bi2O3-CuO-MnO2-Co2O3-Cr2O3压敏陶瓷的正电子寿命谱及其电性能参数。研究了MnO2、Co2O3和Cr2O3掺杂对ZnO-TiO2-Bi2O3-CuO压敏陶瓷电子密度和电性能的影响。实验发现:ZnO-TiO2-Bi2O3-CuOCr2O3压敏陶瓷基体和晶界缺陷态的电子密度均最高,其压敏电压最低;ZnO-TiO2-Bi2O3-CuO-MnO2压敏陶瓷晶界缺陷态的电子密度最低,其压敏电压比前者高;ZnO-TiO2-Bi2O3-CuO-Co2O3压敏陶瓷基体(晶粒内)的电子密度最低,其压敏电压较高;而ZnO-TiO2-Bi2O3-CuO-MnO2-Co2O3-Cr2O3压敏陶瓷基体和晶界缺陷态的电子密度均较低,其压敏电压VT和非线性系数ɑ最高,漏电流IL最小。
简介:Recentadvancesontheuseofnanocarbon-basedelectrodesfortheelectrocatalyticconversionofgaseousstreamsofCO2toliquidfuelsarediscussedinthisperspectivepaper.Anovelgas-phaseelectrocatalyticcell,differentfromthetypicalelectrochemicalsystemsworkinginliquidphase,wasdeveloped.Thereareseveraladvantagestoworkingasphase,e.g.noneedtorecovertheproductsfromaliquidphaseandnoproblemsofCO2solubility,etc.Operatingundertheseconditionsandusingelectrodesbasedonmetalnanoparticlessupportedovercarbonnanotube(CNT)typematerials,longC-chainproducts(inparticularisopropanolunderoptimizedconditions,butalsohydrocarbonsuptoC8-C9)wereobtainedfromthereductionofCO2.Pt-CNTaremorestableandgiveinsomecasesahigherproductivity,butFe-CNT,particularusingN-dopedcarbonnanotubes,giveexcellentpropertiesandarepreferabletonoble-metal-basedelectrocatalystsforthelowercost.ThecontrolofthelocalizationofmetalparticlesattheinneroroutersurfaceofCNTisanimportactfactorfortheproductdistribution.ThenatureofthenanocarbonsubstratealsoplaysarelevantroleinenhancingtheproductivityandtuningtheselectivitytowardslongC-chainproducts.TheelectrodesfortheelectrocatalyticconversionofCO2arepartofaphotoelectrocatalytic(PEC)solarcellconcept,aimedtodevelopknowledgeforthenewgenerationartificialleaf-typesolarcellswhichcanusesunlightandwatertoconvertCO2tofuelsandchemicals.TheCO2reductiontoliquidfuelsbysolarenergyisagoodattempttointroducerenewablesintotheexistingenergyandchemicalinfrastructures,havingahigherenergydensityandeasiertransport/storagethanothercompetingsolutions(i.e.H2).
简介:Cu-Fecompositeoxideswerepreparedbyco-precipitationmethodandtestedforhigheralcoholsynthesisfromsyngas.TheselectivitytoC2+OHandC6+OHinalcoholdistributionwasveryhighwhilethemethaneproductfractioninhydrocarbondistributionwasratherlow,demonstratingapromisingpotentialinhigheralcoholssynthesisfromsyngas.ThedistributionofalcoholsandhydrocarbonsapproximatelyobeyedAnderson-Schulz-Florydistributionwithsimilarchaingrowthprobability,indicatingalcoholsandhydrocarbonsderivedfromthesameintermediates.TheeffectsofCu/Femolarratio,reactiontemperatureandgashourlyspacevelocity(GHSV)oncatalyticperformancewerestudiedindetail.ThesamplewithaCu/Femolarratioof10/1exhibitedthebestcatalyticperformance.Higherreactiontemperatureacceleratedwater-gas-shiftreactionandledtolowertotalalcoholsselectivity.GHSVshowedgreateffectoncatalyticperformanceandhigherGHSVincreasedthetotalalcoholselectivity,indicatingthereexistedvisibledehydrationreactionofalcoholintohydrocarbon.