Partial Oxidation of Methane to Synthesis Gas over (La,Sr)(Co,Ni) Oxide Catalysts.

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  • HAYAKAWA Takashi
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research
  • HARIHARA Hideaki
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research
  • ANDERSEN Arnfinn G.
    Sect. for Hydrocarbon Process Chemistry
  • SUZUKI Kunio
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research
  • YASUDA Hiroyuki
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research
  • SHIMIZU Masao
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research
  • TAKEHIRA Katsuomi
    Dept. of Surface Chemistry, National Institute of Materials and Chemical Research

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  • (La, Sr)(Co, Ni) 酸化物触媒上のメタンの部分酸化による合成ガスの製造
  • Partial Oxidation of Methane to Synthes

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Abstract

The catalytic properties of a series of (La, Sr)(Co, Ni) oxides have been studied for the oxidation of CH4. The catalysts were prepared by the citrate method. The catalytic test using a mixed gas of CH4 and air was carried out by temperature programmed reaction (TPR) from room temperature to 800°C.<br>All the catalysts prepared possessed perovskite oxide structure. The mode of the catalytic oxidation substantially changed around 700°C during the TPR. The oxide catalysts generally catalyzed combustion or oxidative dimerization of CH4 at temperatures below 700°C, while some of the oxides, La1-xSrxNiO3-δ(0≤x≤0.1) and La2-xSrxNiO4-δ(0.1≤x≤1.0), catalyzed synthesis gas production from CH4 at temperatures above 700°C. The latter two oxide catalysts decomposed to form La2O3 and Ni metal after the reaction at 800°C, and the Ni metal seemed to be active species for the synthesis gas formation. However, significant coke formation was observed over the catalysts, resulting in a blockage in the reactor in a short time.<br>LaCoO3-δ was stable and active for the CH4 combustion during the TPR, and showed a very low activity for synthesis gas production at 800°C, where Co metal was not observed. Partial substitution of Sr for La and of Ni for Co, respectively, in LaCoO<sub>3-δ</sub>, i.e., La0.8Sr0.2Co0.8Ni0.2 mixed oxide, resulted in a stable activity for synthesis gas production. The activity was enhanced by pretreating the catalyst, i.e., the reduction with CH4.

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