铜基或锌基二甲醚水蒸气重整制氢高性能催化剂分析-analysis of high performance catalysts for hydrogen production from copper-based or zinc-based dimethyl ether steam reforming.docx

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2018-08-07 发布于上海
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铜基或锌基二甲醚水蒸气重整制氢高性能催化剂分析-analysis of high performance catalysts for hydrogen production from copper-based or zinc-based dimethyl ether steam reforming.docx

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铜基或锌基二甲醚水蒸气重整制氢高性能催化剂分析-analysis of high performance catalysts for hydrogen production from copper-based or zinc-based dimethyl ether steam reforming

ABSTRACTProton-exchangemembranefuelcells(PEMFC)haveattractedmoreandmoreattentionintheresearchareaofelectricvehicles.However,theready-madeH2isveryinconvenientanddangerousforfuelcellapplicationonvehicles.So,itishighlyexpectedthatH2canbeproducedonboard.DMEsteamreforming(DMESR)iseffectiveforhydrogenproductionduetoitsmildreactiontemperatureandhighhydrogenyield.ForDMESR,thedevelopmentofefficientcatalystsisthemostimportant.Inthiswork,thecompositecatalystsofCuorZnbasedoxidecombinedwithsolidacidγ-Al2O3wasemployedforDMESR,theeffectsofpreparationmethod,dopingandcalcinationtemperatureoncatalyticpropertieswereinvestigated,avarietyofcharacterizationmethodswereappliedtoinvestigatethestructuresofthecatalysts.Thepropertiesandstructuresofthecatalystsarewellcorrelated.CitratecomplexmethodwasappliedtopreparetheCuCeOcatalysts,theeffectofMndopingamountonthecatalystwasinvestigated.XRDresultsrevealthatthedopingofMntothecatalystcouldpromotethedispersionofCuspecies.Thecatalystwith5wt%MnexhibitsmoreCu+speciesascomparedwiththeundopedone.ActivitytestsrevealthattheMnsubstitutedCuCeOcatalystsdisplaygoodactivityforDMEconversion;however,itsCO2selectivityisratherlow.TheeffectsofZrdopingandCucontentsontheCuCeOcatalystspreparedbycoprecipitationwerealsoinvestigated.ThedopingofZrcouldincreasetheinteractionbetweenCuandCeZrO,enhancingtheredoxpropertiesofCuspecies.TheoptimalcontentofZrandCuOis10wt%and12wt%,respectively.CuZnAlOcatalystswerepreparedbycoprecipitationmethod,andtheeffectsofZnpartiallysubstitutedbyLaorCeonthecatalyticpropertieswereinvestigated.DopingofasmallamountofLacouldpromotethedispersionofCuspeciesandenhancetheredoxproperties.However,theadditionofexcessLawouldcausetheaggregationofCuspecies.Thecatalystwith3wt%LaexhibitsthehighestspecificsurfaceareaofCuandthebestcatalyticactivity.TheadditionofasmallamountofCecouldreducethegrainsizeofCuandpromotethedispersionofCuandZnO.ExcessamountofCeresultsintheaggregationofCuspecies.Thecatalystwith10wt%CeexhibitsthehighestCudispersionandthebestcatalyticacti