物理化学学报 >> 2014, Vol. 30 >> Issue (10): 1941-1946.doi: 10.3866/PKU.WHXB201408181

催化和表面科学 上一篇    下一篇

Ce0.5Zr0.5O2修饰的Ni/SiC、Fe/SiC和Co/SiC催化燃烧甲烷性能

焦志锋1,2, 董莉莉2, 郭晓宁2, 靳国强2, 郭向云2, 王晓敏1   

  1. 1. 太原理工大学材料科学与工程学院, 太原 030024;
    2. 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 太原 030001
  • 收稿日期:2014-05-14 修回日期:2014-08-11 发布日期:2014-09-30
  • 通讯作者: 郭晓宁, 王晓敏 E-mail:guoxiaoning@sxicc.ac.cn;wangxiaomin@tyut.edu.cn
  • 基金资助:

    山西省自然科学基金（2013021007-1）资助项目

Methane Catalytic Combustion over Ni/SiC, Fe/SiC and Co/SiC Modified by Zr0.5Ce0.5O2 Solid Solution

JIAO Zhi-Feng1,2, DONG Li-Li2,GUO Xiao-Ning2, JIN Guo-Qiang2, GUO Xiang-Yun2, WANG Xiao-Min1   

  1. 1. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, P. R. China;
    2. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China
  • Received:2014-05-14 Revised:2014-08-11 Published:2014-09-30
  • Contact: GUO Xiao-Ning, WANG Xiao-Min E-mail:guoxiaoning@sxicc.ac.cn;wangxiaomin@tyut.edu.cn
  • Supported by:

    The project was supported by the Natural Science Foundation of Shanxi Province, China (2013021007-1).

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摘要：

以铈锆固溶体（Ce0.5Zr0.5O2）修饰的高比表面积SiC为载体，采用两步浸渍法制备了Ni、Fe和Co基催化剂，研究了其在煤层气催化燃烧脱氧中的催化活性和稳定性. 利用X射线衍射（XRD）、X射线光电子能谱（XPS）、电感耦合等离子体质谱（ICP-MS）、高分辨透射电子显微镜（HRTEM）、比表面积（BET）、热重分析（TGA）和H2程序升温还原（H2-TPR）对催化剂进行了表征. 分析结果表明，Ni、Fe和Co部分进入Ce0.5Zr0.5O2固溶体晶格内部，导致催化剂体相形成更多的缺陷；同时Ce0.5Zr0.5O2固溶体有助于加速金属氧化物和金属之间氧化还原过程的进行，促进了氧吸附、传输和对甲烷的活化. 另外，SiC和Ce0.5Zr0.5O2固熔体良好的抗积碳性能，有效避免了催化剂在富甲烷反应气氛中因积碳而失活，从而使三种催化剂均具有优良的催化燃烧脱氧活性和稳定性. 其中，Co/Ce0.5Zr0.5O2/SiC活性最高，可在320 ℃活化催化甲烷，并在410 ℃实现完全脱氧.

关键词: 高比表面碳化硅, 过度金属催化剂, 铈锆固溶体, 甲烷催化燃烧, 煤层气脱氧

Abstract:

We used Zr0.5Ce0.5O2 solid solution modified high specific surface area SiC as the catalyst support and synthesized Ni/Ce0.5Zr0.5O2/SiC, Fe/Ce0.5Zr0.5O2/SiC, and Co/Ce0.5Zr0.5O2/SiC catalysts by a two-step impregnation method. The catalytic activity and stability were investigated in the catalytic combustion deoxidation of coal-bed gas. The as-prepared catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma- mass spectroscopy (ICP- MS), high- resolution transmission electron microscope (HRTEM), Brunner-Emmet-Teller (BET) measurements, thermal gravimetric analysis (TGA), and temperature-programmed reduction of H2 (H2-TPR). The results suggest that partial diffusion of Ni, Fe, and Co to the Ce0.5Zr0.5O2 lattice leads to the formation of defects in the catalyst bulk phase. Ce0.5Zr0.5O2 increased the redox process between metals and their oxides, improving the oxygen storage, mobility capacity, and the activation of CH4. In addition, the excellent resistance of both SiC and Ce0.5Zr0.5O2 solid solution to carbon deposition effectively inhibited coke formation on the catalysts during the combustion of rich methane atmosphere. Hence, these catalysts have good catalytic combustion deoxidation activity and stability. Co/ Ce0.5Zr0.5O2/SiC catalyst had the best activity among the three catalysts: CH4 was activated at 320 ℃ and O2 was completely removed at 410 ℃.

Key words: High surface area SiC, Transition metal catalyst, Zr0.5Ce0.5O2 solid solution, Methane catalytic combustion, Deoxidation of coal-bed gas