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过渡金属氧化物催化CO还原SO2反应的机理

Catalysis Mechanism in Reduction of SO2 by CO over Transition Metal Oxide Catalysts

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【作者】 王广建秦永宁马智胡大为齐晓周

【Author】 WANG Guang-jian, QIN Yong-ning, MA Zhi, HU Da-wei ,QI Xiao-zhou 1. School of Chemical Engineering and Technology, Tianjin University,Tianjin 300072, China; 2. School of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China; 3, Research Institute of Petroleum Processing,Beijing 100083, China

【机构】 天津大学化工学院青岛科技大学化工学院 青岛 266042北京石油化工科学研究院天津 300072北京 100083

【摘要】 采用热重分析、差热分析和光电子能谱对有代表性的Fe、Co和Mo等7种过渡金属催化剂进行表征,研究了Co还原SO2的反应机理和催化剂的催化作用机理及相关的影响因素.结果表明,活性组分不同、负载量相同的催化剂在进行催化反应后表面组成差异较大,S元素的表面分布状态与金属元素密切相关,催化剂表面上金属元素越多,其相应S含量也越高;金属氧化物的硫化路径是先还原后硫化,易于还原的物质更易于硫化;催化活性与空穴分数φd、金属硫化物键能和金属元素的电负性有关,仅从过渡金属的空穴分数φd或各金属硫化物的键能参数难以获得各金属催化剂的催化活性规律,实验表明各金属离子的电负性参数与其催化活性之间存在相关规律.

【Abstract】 The catalytic reduction of SO2 by CO over seven transition metal oxide catalysts was studied by using thermogravimetry(TG) , differential thermogravimetry( DTG) and X-ray photoelectron spectroscopy (XPS). It is found that the catalytic activity of the catalysts investigated is correlated to the electronegativity of the active elements, but not sensitive to the changes in φ_d values of transition metal and bond dissociation energy of metal sulfides. At the same loading, the surface atomic ratio of transition metal and the surface sulfur distribution after reaction vary with the kind of metal. The surface sulfur ratio on catalysts has a direct relation with surface metal atomic ratio. The sulphuration pathway on transition metal oxides is that the metal oxides are firstly reduced and then sulfurized.

【基金】 国家自然科学基金资助项目(90210025;20476048).
  • 【文献出处】 天津大学学报 ,Journal of Tianjin University , 编辑部邮箱 ,2006年04期
  • 【分类号】O643.32
  • 【被引频次】3
  • 【下载频次】379
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