物理化学学报 >> 2012, Vol. 28 >> Issue (05): 1237-1242.doi: 10.3866/PKU.WHXB201203141

催化和表面科学 上一篇    下一篇

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

陈永东1, 王磊2, 唐水花1, 曹红岩3, 龚茂初3, 陈耀强3   

  1. 1. 西南石油大学, 油气藏地质及开发工程国家重点实验室, 成都 610500;
    2. 四川中自尾气净化有限公司, 成都 610225;
    3. 四川大学化学学院, 绿色化学与技术教育部重点实验室, 成都 610064
  • 收稿日期:2011-11-25 修回日期:2012-03-07 发布日期:2012-04-26
  • 通讯作者: 唐水花, 陈耀强 E-mail:shuihuatang@swpu.edu.cn; chenyaoqiang@scu.edu.cn
  • 基金资助:

    国家自然科学基金(21173153)和绿色催化四川省高校重点实验室开放课题基金(LYY1101)资助项目

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-Dong1, WANG Lei2, TANG Shui-Hua1, CAO Hong-Yan3, GONG Mao-Chu3, CHEN Yao-Qiang3   

  1. 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
  • Received:2011-11-25 Revised:2012-03-07 Published:2012-04-26
  • Contact: TANG Shui-Hua, CHEN Yao-Qiang E-mail:shuihuatang@swpu.edu.cn; chenyaoqiang@scu.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21173153) and Opening Project of Key Laboratory of Green Catalysis of Sichuan Institutes of High Education, China (LYY1101).

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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 °C起燃, 553 °C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

Abstract: Ce0.45Zr0.45Y0.07La0.03O1.95, an oxygen storage material (OSM), and La-Ba-Al2O3 have been prepared by co-precipitation and peptization, respectively, to be used as supports for Fe2O3 catalysts. The Fe2O3 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-Al2O3 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 H2-temperature-programmed reduction (H2-TPR). The highest catalytic activity of both fresh and aged Fe2O3 catalysts for thin methane combustion was observed when the mass ratio of OSM/La-Ba-Al2O3 was 1:1. At this OSM/La-Ba-Al2O3 mass ratio, methane started to convert at 446 °C and completely converted at 553 ° C, with 1% (volume fraction) CH4 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-Al2O3 had different specific surface areas and reducibilities. XRD results showed that OSM existed in uniform solid solution and Fe2O3 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-Al2O3 for thin methane combustion.

Key words: Fe2O3 based monolithic catalyst, OSM/La-Ba-Al2O3 mass ratio, Catalytic combustion of thin methane

MSC2000: 

  • O643