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Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比对整体式铁基催化剂上稀薄甲烷燃烧的影响
引用本文:陈永东,王磊,唐水花,曹红岩,龚茂初,陈耀强.Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比对整体式铁基催化剂上稀薄甲烷燃烧的影响[J].物理化学学报,2012,28(5):1237-1242.
作者姓名:陈永东  王磊  唐水花  曹红岩  龚茂初  陈耀强
作者单位:1. State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, P. R. China; 2. Sichuan Zhongzi Exhaust Purge Co., Ltd., Chengdu 610225, P. R. China; 3. Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China
基金项目:国家自然科学基金,绿色催化四川省高校重点实验室开放课题基金
摘    要:采用共沉淀法和胶溶法分别制备了高性能的储氧材料Ce0.45Zr0.45Y0.07La0.03O1.95(OSM)和耐高温高比表面的La-Ba-Al2O3,并以它们为载体,制备了一系列整体式铁基催化剂.考察了该系列催化剂对甲烷稀薄燃烧的催化性能.并用低温N2吸附-脱附,储氧量(OSC)测试,X射线衍射(XRD)和H2程序升温还原(H2-TPR)等测试手段考察了不同Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比对催化剂特性的影响.活性测试结果表明,当Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比为1:1时新鲜和老化催化剂的活性均最好,新鲜催化剂可在50000h-1的高空速条件下使含量为1%(体积分数)的甲烷在446℃起燃,553℃完全转化;低温氮气吸附-脱附测试结果和H2-TPR表明,不同的Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比使催化剂表现出不同的织构性能和还原性能;XRD测试结果表明,OSM以均一固溶体存在,Fe高度分散在载体上.综合以上表征手段得出:合适的Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3质量比导致催化剂具有优异的稀薄甲烷催化燃烧活性和热稳定性.

关 键 词:Fe2O3基整体式催化剂  OSM/La-Ba-Al2O3质量比  稀薄甲烷催化燃烧  
收稿时间:2011-11-25
修稿时间:2012-03-14

Effect of Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3 Mass Ratio on the Activity of Fe-Based Monolithic Catalysts for the Combustion of Thin Methane
CHEN Yong-Dong , WANG Lei , TANG Shui-Hua , CAO Hong-Yan , GONG Mao-Chu , CHEN Yao-Qiang.Effect of Ce0.45Zr0.45Y0.07La0.03O1.95/La-Ba-Al2O3 Mass Ratio on the Activity of Fe-Based Monolithic Catalysts for the Combustion of Thin Methane[J].Acta Physico-Chimica Sinica,2012,28(5):1237-1242.
Authors:CHEN Yong-Dong  WANG Lei  TANG Shui-Hua  CAO Hong-Yan  GONG Mao-Chu  CHEN Yao-Qiang
Institution:1. State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, P. R. China; 2. Sichuan Zhongzi Exhaust Purge Co., Ltd., Chengdu 610225, P. R. China; 3. Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China
Abstract:Ce 0.45 Zr 0.45 Y 0.07 La 0.03 O 1.95,an oxygen storage material(OSM),and La-Ba-Al 2 O 3 have been prepared by co-precipitation and peptization,respectively,to be used as supports for Fe 2 O 3 catalysts.The Fe 2 O 3 catalysts were obtained by impregnation methods and then coated on the monolith.The catalytic combustion of low concentration(thin)methane was investigated over the prepared catalysts.The effect of the OSM/La-Ba-Al 2 O 3 mass ratio on the physicochemical properties of the catalysts was investigated using nitrogen adsorption-desorption,oxygen storage capacity(OSC)measurements,X-ray diffraction(XRD),and H 2-temperature-programmed reduction(H 2-TPR).The highest catalytic activity of both fresh and aged Fe 2 O 3 catalysts for thin methane combustion was observed when the mass ratio of OSM/La-Ba-AL 2 O 3 was 1:1.At this OSM/La-Ba-AL 2 O 3 mass ratio,methane started to convert at 446℃ and completely converted at 553℃,with 1%(volume fraction)CH 4 and a gas hourly space velocity(GHSV)of 50000 h-1.The Fe-based monolithic catalysts with different mass ratios of OSM to La-Ba-Al 2 O 3 had different specific surface areas and reducibilities.XRD results showed that OSM existed in uniform solid solution and Fe 2 O 3 was well dispersed on the binary supports.Based on the characterizations,the high catalytic activity and thermal stability of the catalysts can be attributed to the proper coordination of OSM and La-Ba-AL 2 O 3 for thin methane combustion.
Keywords:Fe2O3 based monolithic catalyst  OSM/La-Ba-Al2O3 mass ratio  Catalytic combustion of thin methane
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