甲烷-合成气两步梯阶反应合成乙酸的反应机理

项目名称： 甲烷-合成气两步梯阶反应合成乙酸的反应机理

项目编号： No.21276003

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 化学工业

项目作者： 章日光

作者单位： 太原理工大学

项目金额： 80万元

中文摘要： 青年科学基金已确定了一套能够准确描述CH4-CO2两步梯阶反应合成乙酸热力学、动力学的金属催化剂反应模型及方法，包括CHx与金属表面、CHx和H分别与CO2作用以及CHx溢流对两步梯阶反应的影响；并获得等温下两步梯阶反应合成乙酸适宜的金属催化剂，且部分催化剂已被实验证实具有较好催化性能，研究结果可为新型催化剂的筛选和设计提供比较准确的指导方案；依据青年科学基金研究结果，发表SCI收录论文16篇。同时，青年科学基金研究表明CO2与H作用容易生成CO和OH，结合实验产物没有检测到CO这一事实，认为CO插入CHx并与OH作用形成CHxCOOH，进而加氢生成乙酸；因此，本项目提出甲烷-合成气两步梯阶反应合成乙酸的研究，采用量子化学计算和实验相结合的方法，从催化剂构效关系、反应热力学和动力学方面阐明金属催化剂作用下甲烷-合成气两步梯阶反应合成乙酸的反应机理，为实验筛选并提出适宜的金属催化剂。

中文关键词： 甲烷；合成气；乙酸；反应机理；密度泛函理论

英文摘要： In NSFC, a set of metal catalyst models and methods has been established, including the mechanisms of CHx interaction with metal surface, CHx interaction with CO2, as well as the effect of CHx overfall on two-step reactions, which can be applied to accurately describe the reaction thermodynamics and kinetics for CH4-CO2 two-step synthesis to form acetic acid. Moreover, the most suitable metal catalysts for two-step synthesis to acetic acid have been obtained; further, these catalysts have been experimentally verified with good catalytic properties, suggesting that our research results can provide more accurate prediction schemes for the filtration and design of new catalysts. According to the results of NSFC, sixteen papers indexed by SCI have been published. Meanwhile, an interesting result in NSFC shows that the interaction of CO2 with H can easily generate CO, combining with the experimental fact that CO has not been detected in products, as a result, it is thought that CO involves in the two-step reaction to form acetic acid, in which CHx interacts with CO and OH to form an intermediate CHxCOOH, then, the hydrogenation of CHxCOOH leads to CH3COOH; therefore, the idea of methane-synthesis gas by two-step methods to produce acetic acid is proposed. By using quantum chemical DFT theoretical calculations combini

英文关键词： methane；syngas；acetic acid；mechanism；density functional theory