Chinese Journal of Catalysis ›› 2014, Vol. 35 ›› Issue (1): 8-20.DOI: 10.1016/S1872-2067(12)60723-2

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Preparation and characterization of Ni/CeO2-SiO2 catalysts and their performance in catalytic partial oxidation of methane to syngas

Jiubiao Hua, Changlin Yua, Yadong Bib, Longfu Weia, Jianchai Chena, Xirong Chena   

  1. a School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiangxi, China;
    b School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China
  • Received:2013-07-23 Online:2013-12-23 Published:2014-01-17
  • Contact: Changlin Yu, Yadong Bi
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21067004, 21263005, 21003095), Science and Technology Foundation of Jiangxi Provincial Department of Education (GJJ12344), Program of Jiangxi Provincial Young Scientists Cultivating Object (20122BCB23015), and Young Science and Technology Project of Jiangxi Province Natural Science Foundation (20133BAB21003).

Abstract:

Hexahydrated cerium(Ⅲ) nitrate (Ce(NO3)3·6H2O) and tetraethyl orthosilicate (C8H20O4Si) were used as the precursors for the synthesis of a series of xCeO2-(1-x)SiO2 (x = 0, 0.25, 0.5, 0.75, 1) composite oxides using a sol-gel process under acidic conditions. The active component, Ni, was loaded on the as-synthesized composite oxides, producing supported Ni catalysts for catalytic partial oxidation of methane to syngas. The properties of the as-synthesized products, such as textural structure, reduction behavior, surface acidity, and carbon deposition, were determined using N2 physical adsorption/desorption, X-ray diffraction, scanning electron microscopy, ultraviolet-visible diffuse reflectance spectroscopy, temperature-programmed reduction by H2, temperature-programmed desorption of NH3, and thermogravimetric analysis. The effects of catalyst composition, calcination temperature, and reaction time on the catalytic performance were investigated. The characterization results showed that these Ni/CeO2-SiO2 catalysts have large surface area, small CeO2 crystals, weak acidity, and low carbon deposition. Highly dispersed NiO is present and is easy to be reduced. The Ni/CeO2-SiO2 catalyst with a Ce/Si molar ratio of 1:1, w(Ni) = 10%, and calcined at 700℃ exhibited good stability and the highest CH4 conversion (~84%) and CO and H2 selectivity (> 87%).

Key words: Sol-gel process, Ceria-silica composite oxide, Supported nickel catalyst, Partial oxidation of methane, Syngas