Ni金屬基整體型催化劑催化甲烷轉(zhuǎn)化制備合成氣的研究.pdf

1、天津大學(xué)博士學(xué)位論文Ni金屬基整體型催化劑催化甲烷轉(zhuǎn)化制備合成氣的研究姓名：李云華申請學(xué)位級別：博士專業(yè)：化學(xué)工藝指導(dǎo)教師：王亞權(quán)20061201天津大學(xué)博士論文ABSTRACTMethanepartialoxidationtosyngasisoneofthepromisingwaystOefficientlyutilizemethaneBecauseofitslowinvestmentandenergyconsumptionwithi

2、nstantreactionrate，ithasattractedmuchattentionInthepresentwork，NimetallicmonolithcatalystwaspreparedwithNifoamandfurthertreatedbyacidItWas10adedbypromoteroxides，suchasceria，zirconia，magnesia，ceriazirconia，etc，toobtainthe

3、Nimonolithwithoxides乃esamplecharacterizationwasmadebyXRDlXPS、SEM、ICPandBETConsideringthatthedeactivationoftheNimetallicmonolithcouldnotoccurandithadloweractivitythanthesupportedcatalysts，thedualbed，NimonolithNi／MgAl204，w

4、asalsostudiedformethanepartialoxidationMoreover，onthebasisofanindirectreactionmechanism，simulationsofmethanepartialoxidationwereconductedforthesethreekindsofcatalystsystemsSEMmicrographsshowedthatthecrystaldefectsonthesu

5、rfaceoftheNimonolithwereformedThesurfaceareaincreasedfrom03m2／gofuntreatedNimonolithto05m2／gof也eNimonolithtreatedbyacidAtinlettemperature1123K，CH4／02ratioof2andGHSV1Ox105h1，methaneconversionandselectivitiestoH2andCOonthe

6、Nimonolithtreatedbyacidwere90％，98％and95％，respectively，muchhigherthanthoseoftheuntreatedNimonolith，whichwere84％，92％and94％，respectivelyTheoptimalloadingsofceriaandzirconia，separately，were287％and157％，respectivelyTheoptimall

7、oadingofmagnesiaWas403％whilecalciumoxidehadnoleforpromotionoftheactivityandtheselectivities087％Ce一177％Zr／Nishowednotonlyhighactivityandselectivities，butalsohighstability。XRDpaRernsshowedthatCe02一Zr02solidsolutionWasforme

8、don087％Ce一177％Zr／NiTheresultsshowedthatthereactionperformanceforthecombinedpartialoxidationandsteamreformingofmethanewasbetterthanthecombinedpartialoxidationandcarbondioxidereformingofmethaneonbothCe—Zr／NimonolithandMg／N

9、iThedualbed，NimonolithNi／MgAl204，hadthehighestactivityandselectivitieswhenthenickelloadingonthereformingcatalystWaslOwt％Theresultsshowedthatwhenthefeedflowrateswere500ml／minor1000ml／min。23or47mmoftheminimumlengthoftheNim