溶液燃烧法制备的Ni基催化剂及其浆态床甲烷化催化性能.pdf

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1、第31卷第2期无机化学学报Vo1．31No．22015年2月CHINESEJOURNALOFIN0RGANICCHEMISTRY267—274溶液燃烧法制备的Ni基催化剂及其浆态床甲烷化催化性能吉可明盂凡会高源李忠(太原理工大学，煤科学与技术教育部和山西省重点实验室．太原030024)摘要：分别以硝酸铝、硝酸氧锆、硝酸镧和硝酸铈为载体前驱体，与硝酸镍和尿素配制水溶液，采用溶液燃烧法制备了Ni—A1，O、Ni—ZrOz、Ni—La2O和Ni—CeO：催化剂，研究了浆态床C0甲烷化催化性能，并进行了低温N吸附一脱附、XRD、SEM、TEM、H，TPR和H：化学吸附等表征分析。结

2、果表明，以硝酸铝为前驱体制备M—Al20催化剂时燃烧火焰稳定且持续时间长．达23s．样品比表I~R(468m2og)和金属Ni表面积(10m2og)均较大、Ni粒径小(3—5nm)且分散度高，C0甲烷化催化活性和稳定性好．C0转化率和CH选择性分别达到94％和95％，在100h的甲烷化反应中未出现明显失活；以硝酸氧锆和硝酸镧为前驱体制备样品时未出现明显的燃烧火焰，持续时间仅为12s和5s，催化剂比表面积、金属表面积及催化活性均较低：以硝酸铈为前驱体制备样品时燃烧过程迅速而剧烈，样品比表面积(22ITI2~g。)和金属表面积(5m·g一)小、Ni粒径大且分散性差，甲烷化催化性

3、能最差．CO转化率仅为41％．CH选择性仅为89％关键词：催化；催化剂制备；浆态床反应器；c0甲烷化；溶液燃烧法；镍催化剂；载体中图分类号：0614；0643．3文献标识码：A文章编号：1001—4861(2015)02—0267—08DoI：10．11862／CJIC．2015．050SolutionCombustionPreparedNi-BasedCatalystsandTheirCatalyticPerformanceforSlurryMethanationJIKe—MingMENGFan—HuiGAOYuanLIZhong(KeyLaboratoryofCoalS

4、cienceandTechnologyofMinistryofEducationandShanxiProvinceTaiyuanUniversityofTechnology,Taiyuan030024,China)Abstract：Ni—A1203，Ni-ZrO2，Ni—La203andNi—CeO2catalystswerepreparedbysolutioncombustionmethodusingA1(NO3)3，ZrO(NO3)2，La(NO3)3andCe(NO3)3(mixedwithNi(NO3)2andureainaqueoussolution)asthes

5、upportprecursor，respectively．TheCOmethanationperformancesofcatalystswerestudiedinslurry—bedreactor．andthecatalystswerecharacterizedbylowtemperatureN2adsorption—desorption，XRD，SEM，TEM，H2．TPRandH2chemsorption．TheresultsshowthatthecombustionpreparationprocessofNi—A1203catalystusingAI(NO3)2ast

6、heprecursorisstableforlong—duration(upto23S)andthecatalysthaslargersurfacearea(468m·g)andmetalsurfacearea(10mg-1)，smallerNiparticle(3-5nm)，excellentdispersionofNi，andthecatalysthasgoodcatalyticperformance，whoseCOconversionandCH4selectivityare94％and95％，respectivelv。andnocatalystdeactivation

7、isobservedin100h．ThepreparationprocessforcatalystsusingZrO(N03)2andLa(NO3)3asprecursorsdoesnotshowobviousflameandburningtimeisalsoshorter(12Sand5s1，thesurfaceareasmetalsurfaceareasandcatalyticperformancesarelowerthanthatofNi-A12O3whilethatf0rthecatalystusingCe