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Modified Ceria-Zirconia Fluorite-Like Catalysts for the Combustion of Methane
作者姓名:Tatiana  Kuznetsova  Vladislav  Sadykov  Lubsan  Batuev  Ella  Moroz  Elena  Burgina  Vladimir  Rogov  Vladimir  Kriventsov  Dmitrii  Kochubey
作者单位:Boreskov Institute of Catalysis SB RAS Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia,Boreskov Institute of Catalysis SB RAS,Pr. Lavrentieva,5,Novosibirsk,630090,Russia
基金项目:Acknowledgements This work is supported in part by the ISTC 3234 and RFBR-CNRS 05-03-34761 projects.
摘    要:For dispersed ceria-zirconia-based solid solutions prepared via the polymerized complex method and annealed at 700℃, effects of bulk doping by Ca, Mn, Co, Bi or Nb cations and surface modification by Mn and Pt on their structural features, surface/bulk oxygen reactivity and catalytic activity in methane combustion are considered. With up to 20 mol% doping, a structural type of homogeneous solid solutions of anion-deficient fluorite with disordered anion vacancies is formed. Doping by transition metal cations or Pt increases the mobility and reactivity of the surface/bulk oxygen. A broad variation in specific rates of methane combustion for the studied systems was observed, suggesting structural sensitivity of this reaction. In general, there is no universal relationship between the oxygen mobility, the reactivity and the catalytic activity in methane combustion, which is explained by the factor of specific methane activation on surface active sites. For the Pt-promoted samples, Pt efficiency in methane activation depends on the Pt-support interaction, and the most favorable ones being mixed Pt/MnOx and Pt/NbOx clusters on the surface of the supports that exhibit high lattice oxygen mobilities.

关 键 词:Ce-Zr-O  Ca  Mn  Co  Bi  Nb  催化剂  结构表征  氧反应  氧迁移率  甲烷燃烧
收稿时间:03 14 2006 12:00AM
修稿时间:04 24 2006 12:00AM

Modified Ceria-Zirconia Fluorite-Like Catalysts for the Combustion of Methane
Tatiana Kuznetsova Vladislav Sadykov Lubsan Batuev Ella Moroz Elena Burgina Vladimir Rogov Vladimir Kriventsov Dmitrii Kochubey.Modified Ceria-Zirconia Fluorite-Like Catalysts for the Combustion of Methane[J].Journal of Natural Gas Chemistry,2006,15(3):149-163.
Authors:Tatiana Kuznetsova  Vladislav Sadykov  Lubsan Batuev  Ella Moroz  Elena Burgina  Vladimir Rogov  Vladimir Kriventsov  Dmitrii Kochubey
Institution:Boreskov Institute of Catalysis SB RAS, Pr. Lavrentieva, 5, Novosibirsk, 630090, Russia
Abstract:For dispersed ceria-zirconia-based solid solutions prepared via the polymerized complex method and annealed at 700 ℃, effects of bulk doping by Ca, Mn, Co, Bi or Nb cations and surface modification by Mn and Pt on their structural features, surface/bulk oxygen reactivity and catalytic activity in methane combustion are considered. With up to 20 mol% doping, a structural type of homogeneous solid solutions of anion-deficient fluorite with disordered anion vacancies is formed. Doping by transition metal cations or Pt increases the mobility and reactivity of the surface/bulk oxygen. A broad variation in specific rates of methane combustion for the studied systems was observed, suggesting structural sensitivity of this reaction. In general, there is no universal relationship between the oxygen mobility, the reactivity and the catalytic activity in methane combustion, which is explained by the factor of specific methane activation on surface active sites. For the Pt-promoted samples, Pt efficiency in methane activation depends on the Pt-support interaction, and the most favorable ones being mixed Pt/MnOx and Pt/NbOx clusters on the surface of the supports that exhibit high lattice oxygen mobilities.
Keywords:Ce-Zr-O  Ca  Mn  Co  Bi  Nb  structural features  oxygen reactivity  oxygen mobility  methane combustion
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