物理化学学报 >> 1996, Vol. 12 >> Issue (08): 741-745.doi: 10.3866/PKU.WHXB19960813

研究论文 上一篇    下一篇

担载型贵金属催化剂上甲烷直接羰基化反应

阎子峰,薛锦珍,沈师孔,王弘立   

  1. 石油大学炼制系，山东东营 257062|中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室，兰州 730000
  • 收稿日期:1996-01-03 修回日期:1996-05-10 发布日期:1996-08-15
  • 通讯作者:

Studies of Direct Carbonylation of Methane on Supported Transition Metal Catalysts

Yan Zi-Feng,Xue Jin-Zhen,Shen Shi-Kong,Wang Hong-Li   

  1. Department of Chemical Engineering,University of Petroleum,Dongying 257062|State Key Laboratory of Oxo Synthesis and Selective Oxidation,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 730000
  • Received:1996-01-03 Revised:1996-05-10 Published:1996-08-15
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摘要：

利用程序升温脉冲反应、恒温脉冲反应及探针分子表面反应技术较系统地考察了担载型贵金属催化剂上甲烷直接羰基化制乙醛的反应，研究发现通过采用总反应分解法操作后，能够克服甲烷直接羰基化反应的热力学限制，将总反应转化为两个可在较温和条件发生的反应，首次实现了CH4＋CO→CH3CHO的反应. 即首先进行甲烷的分解，然后引入CO与甲烷分解所产生的表面物种直接反应生成乙醛．本文还探讨了甲烷吸附条件，CO与甲烷分解所产生的表丙碳物种间的作用等反应的影响因素. 探针分子CH3I的表面反应结果显示甲烷分解产生的CHx（ad）（x≤3）物种可能是该反应的活性中间体.

Abstract:

Direct carbonylation of methane on silica-supported noble metal catalysts was tentatively investigated by using temperature programmed pulse reaction (TPPR), constant temperature pulse reaction (CTPR) and surface reaction of probe molecules CH3I (SRPM). An important approach is to split the overall reaction into two reaction steps occurring under moderate conditions. Methane decomposition on transition metal surface was first employed to form surface carbonaseous species. Then CO was introduced to interact with surface carbonaceous species to produce aldehyde. In such a two-step route the thermodynamic limitations can be overcome and the direct carbonylation of methane may be effectively achieved. This reaction is an attractively novel route for the utilization of methane. Optimization of this process might result in a new route for effective ultilization of methane.

Key words: Carbonylation of methane, Noble metals catalysts, Ethanal formation