CH_2c4_2fCO_2c2_重整反应镍基催化剂上积碳机理分析

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1、MechanisticstudiesofcarbondepositionOilNi—basedcatalystsduringmethanereformingwithcarbondioxideWu，Pingping(IndustrialCatalysis)DirectedbyProfessorYah，ZifengAbstractCarbondepositiononcatalystsisahauntingproblemformethanereformingwithcarbondioxide，whichisthereasonthatthisprocessisdifficulttobecommerci

2、alized．Sostudyonthemechanismofcarbondepositionduringmethanereformingwithcarbondioxidehasrecentlyreceivedanincreasinginterest．Themainpurposeofthispaperistochooseacatalystwithsuperioractivityandselectivity,andinvestigatetherulesandmechanismofcarbondepositiononit,thenthroughcatalystdesignandreactioncon

3、ditionsoptimizationtoobtainabalancebetweencarbonformationandremoval，andeventuallytoprohibitthecarbondepositionfromdeactivatingthecatalysts．Inthispaper,theinfluenceofdifferentsupportsynthesismethods，differentcatalystspreparationmethodsanddifferentpromotersontheperformanceofcatalystswasinvestigated；th

4、eresultsshowedthatthecatalystbyusingZr02synthesizedbysolid-statemethodassupport,Ce02aspromoterandpreparedbystep—impregnationmethodexhibitedthebestreactionperformance．ItWasduetothefactthatZr02synthesizedbysolid·statemethodhasexcellentstructureproperties，suchaslargeBETsurfaceareaandnarrowporesizedistr

5、ibution，whichWasbenefittothedispersionofactivecomponent(Ni)andalsoitsnano-sizeeffectenhanceedthecatalystactivity．StepwisedimpregnationfavorsthedispersionofNionthesupport,andtheintroductionofCe02asapromoterstrengthensthe02removalabilityofthecatalyst，whichincreasestheresistancetocarbondepositiononit．A

6、fteroptimizingthecatalystsystem，therulesandmechanismofcarbondeposition011Ni-Ce02／Zr02wereinvestigated．TG—DTA，SEMandTEM-EDSwereutilizedtocharacterizethecarbonspeciesandcarbonmorphologyonspentcatalysts．Theresultsshowedthatthereweretwokindsofcarbondepositsonspentcatalyst卜——aIllorphouscarbonandcarbonnan

7、otube(CNT)．TheformationofdifferentcarbonmorphologiesWascontrolledbykineticsandwasindependentofcarbonsources．OnNi—Ce02／Zr02catalyst，twoChITgrowthmechanismsexistatthesametime———-——basegrowthmechanismand