合成气直接制高碳混合醇双活性位催化剂的设计及构效关系研究

The direct conversion of syngas into long-chain alcohols（C6+OH）is very attractive in modern coal chemical industry due to its simplified process and high economic value. The main challenge is to increase long chain alcohols selectivity through catalyst design. Co/MnOx nanocatalyst with high dispersion and rich boundaries for long-chain alcohols synthesis via syngas will be developed in this project. The highly dispersed Co will increase the ability of the carbon chain growth and the rich contact boundaries between active sites would enhance the synergism effect and thus improve C6+OH selectivity. The structure-performance relationship will be discussed based on the correlation between structure evolution and the change of catalytic performance, and theoretical computation. The synergism effect on C-O activation and cleavage, carbon chain growth and the nature of the active site benefited for long chain alcohols formation will be clarified. The implement of this project will deep the understanding of dual active sites in the Co/MnOx catalyst and will provide theoretical basis and valuable information for the design of C6+OH catalysts with high activity and selectivity.

由合成气直接制备高碳醇（C6+OH）路线短、产品附加值高，是极具经济价值的现代煤化工技术之一。如何通过催化剂的构筑提高对高碳醇的选择性是目前该课题的研究关键。在本项目中，我们将围绕合成气制高碳醇反应，设计高分散、高接触面的Co/MnOx纳米催化剂，提高催化剂链增长能力同时增加双活性界面效应。同时，围绕高碳醇选择性控制的本质原因，结合相关的表征手段及理论计算，开展深入的构效关系研究，了解双活性位相互作用对CO活化、链增长等反应过程的影响，揭示出高碳醇形成的本征活性位，从而为高活性、高选择性的合成气制高碳醇催化剂的开发提供理论基础和指导。

由合成气直接制备高碳醇（C6+OH）路线短、产品附加值高，是极具经济价值的现代煤化工技术之一。在本项目中，我们围绕合成气制高碳醇反应，以层状结构为前驱体，制备了高分散、高接触面的Co/MnOx纳米催化剂，提高催化剂链增长能力同时增加双活性界面效应。同时，围绕高碳醇选择性控制的本质原因，结合原位和离线的表征手段及开展深入的构效关系研究，了解双活性位相互作用对CO活化、链增长等反应过程的影响，发现Co2C/Co 的晶界面和 Co2C 的不同暴露晶面的晶界面是 CoMn 催化剂的混合醇合成双活性位点，从而为高活性、高选择性的合成气制高碳醇催化剂的开发提供理论基础和指导。