W-Mn/SiO _2甲烷氧化偶联催化剂流化床的放大研究

在催化剂装量为２００ｍＬ的不锈钢流化床反应器上，Ｗ－Ｍｎ／ＳｉＯ２催化剂甲烷氧化偶联反应性能及稳定性试验结果表明，在甲烷空速为７０００ｈ－１，反应温度为８００℃，原料中氧含量为１１．８％时，Ｃ２烃选择性和收率分别可达８２．６％和１７．８６％；反应温度为８７５℃，Ｏ２含量为１５．１％时，Ｃ２烃收率和选择性分别为１９．４％和７５．７％。在４５０ｈ稳定性试验中，Ｃ２烃的收率和选择性一直在１７％和７０％以上。另外，用ＸＲＤ、ＩＣＰ－ＡＥＳ和ＢＥＴ等手段分别对新鲜催化剂和经稳定性试验后的催化剂进行了表征。

OxiditiveCouplingofMethaneoverW┐Mn/SiO2CatalystinaBench┐ScaleStainlesStelFluidized┐BedReactorWangXiaolai,ZhangJianing,YangDexin,ZhangChuanwei,LinJingzhiandLiShuben(NationalEngineringResearchCenterforFinePetrochemicalIntermediates,LanzhouInstituteofChem

heoxidativecouplingofmethanetohigherhydrocarbonsoverW-Mn/SiO2catalysthasbeenconductedinastainlesssteelfluidized-bedreactorwhichcontained200mL(130g)catalyst.Theinfluencesofthefeedgasoxygenlevel,temperatureandmethanespacevelocityonC2selectivityandyieldwerestudied.ThehighestC2yieldachieved19.4%atmethaneconversionof25.6%,whilemaximumselectivityof82.6%wasobtainedatmethaneconversionof21.6%.Thestabilitytestforthecatalystwasalsoperformed,andduringaperiodof450h,bothC2selectivityandyieldwerehigherthan70.0%and17.0%respectively.Freshcatalystsandthoseafter450hstabilitytestwerecharacterizedbyXRD,ICP-AESandBET.Abstract The oxidative coupling of methane to higher hydrocarbons over W Mn/SiO 2 catalyst has been conducted in a stainless steel fluidized bed reactor which contained 200mL(130g) catalyst The influences of the feed gas oxygen level,temperature and methane space velocity on C 2 selectivity and yield were studied The highest C 2 yield achieved 19 4% at methane conversion of 25 6%,while maximum selectivity of 82 6% was obtained at methane conversion of 21 6% The stability test for the catalyst was also performed, and during a period of 450h,both C 2 selectivity and yield were higher than 70 0% and 17 0% respectively Fresh catalysts and those after 450h stability test were characterized by XRD,ICP AES and BET