Cu基催化剂作用下甲烷-合成气定向合成乙醇的构效关系

项目名称： Cu基催化剂作用下甲烷-合成气定向合成乙醇的构效关系

项目编号： No.21476155

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 有机化学

项目作者： 章日光

作者单位： 太原理工大学

项目金额： 87万元

中文摘要： 合成气合成乙醇是煤化工过程中的一个重要反应，但该反应乙醇产率较低；然而，合成气中引入甲烷，通过全新反应机理的甲烷-合成气合成乙醇的新方法是解决乙醇产率的可行途径，能够实现生成乙醇关键步骤的改变。本项目采用量子化学理论计算、实验表征和催化性能评价等3种手段相结合的方法，在电子水平上明确Cu基催化剂作用下的甲烷-合成气定向合成乙醇的催化反应动力学机理，阐明金属掺杂、载体调变Cu基催化剂的组成、比例、颗粒大小和表面结构等主要结构因素与定向合成乙醇催化性能(活性、选择性和稳定性)的构效关系；获得调控负载型Cu基双金属催化剂催化性能的理论和方法；建立反应动力学微观参量与催化剂宏观可评价性能的关系；在工艺实践方面，为甲烷-合成气定向合成乙醇反应中Cu基催化剂的筛选和改性，以及有针对性地设计新型高效Cu基催化剂，提供基本的理论线索和操作方案。

中文关键词： Cu基催化剂；甲烷；合成气；乙醇；构效关系

英文摘要： Ethanol synthesis from syngas is an important reaction in the process of coal chemical industry, but the yield of ethanol is low; by the introduction of methane into syngas, a completely new reaction mechanism of ethanol synthesis via methane-syngas routes can be applied to imporve the ethanol yield, which can realize the change of key rate-controlling step for the catalytic reaction of ethanol synthesis; Based on quantum chemical calculations combined with the experimental characterization and catalytic performance evaluation methods, the kinetics mechanism of catalytic reaction of methane-syngas to ethanol on Cu-based catalyst are expected to be clarified at the electronic level, and the structure-activity relationship of the catalysts between the structural factors and catalytic performacne(activity, selectivity and stability) can be illustrated, in which the structural factors of Cu-based catalyst with different composition, proportion, particle size and surface morphology are adjusted by the metal-doping and support. Meanwhile, the theory and method to modulate the catalytic performance of the supported Cu bimetallic catalyst can be established; further, the relationship between the micro-parameters of reaction kinetics and the macro-evaluable properties of catalysts can be obtained. Finally, in the practical process of methane-syngas to ethanol, for the filtration and modification of Cu-based catalysts, as well as to the design of new efficient Cu-based catalyst, the theoretical clues and basic operation scheme can be obtained.

英文关键词： Cu-based catalyst;methane;syngas;ethanol;Structure-activity relationship