Acta Phys. -Chim. Sin. ›› 2014, Vol. 30 ›› Issue (10): 1941-1946.doi: 10.3866/PKU.WHXB201408181

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

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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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