高选择性过渡金属碳化物/氧化物催化加氢机理的研究及催化剂的设计与制备

项目名称： 高选择性过渡金属碳化物/氧化物催化加氢机理的研究及催化剂的设计与制备

项目编号： No.21473164

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 程寒松

作者单位： 中国地质大学（武汉）

项目金额： 84万元

中文摘要： 异相催化加氢在石油化工、制药等领域有着非常广泛的应用。然而，依赖于贵金属催化剂的加氢反应过程存在选择性不够高、催化剂易中毒等缺陷。本项目提出基于廉价金属氧化物/碳化物的选择性加氢催化剂，不仅具有与贵金属相当的催化加氢活性，而且具有优秀的选择性和抗毒性。项目采用计算设计先行，实验制备、检测与之相互反馈、相互验证的技术路线，通过系统的研究基于廉价金属氧化物/碳化物催化剂对不饱和分子的加氢行为，获得其催化反应机理；通过研究具有不同结构特征的催化剂的催化行为，揭示催化剂的结构特征对其催化活性、选择性及抗毒性的影响规律；最终优化设计并制备一系列针对指定特征基团具有最佳催化性能的新型催化剂，为我国石油化工及生物制药中分子的不饱和键的选择性催化加氢提供理论和技术支持。

中文关键词： 催化机理；选择性加氢；过渡金属碳化物；过渡金属氧化物；氢溢流

英文摘要： Heterogeneous catalytic hydrogenation is widely used in petrochemical and pharmaceutical processes. However, many of the processes are largely based on noble metal catalysts, which suffer from relatively poor selectivity and catalyst poisoning. Here, we propose a class of inexpensive metal oxides/carbides as potenential but promising catalysts for selective heterogeneous hydrogenation. These materials were found to have comparable catalytic activity to that of noble metals for hydrogenation with superior selectivity and more resistant to catalyst poisoning. The proposed research will employ the state-of-the-art first principles based methods to calculate the thermochemical, kinetic and dynamic properties of various hydrogenation process and to guide our experimental work to design and discover new catalysts. Particular research emphasis will be placed on the fundamental understanding of hydrogenation mechanisms based on the selected metal oxides/carbides. We will unravel the atomistic detalis of the hydrogenation process and the fundamental relationship etween catalyst' structure and reactivity and selectivity. Issues related to catalyst poisoning will be addressed through comparison studies between the chosen catalysts and the conventional precious metal based catalysts using first principles calculation and a variety experimental techniques. A series of catalysts with high selectivity and high efficiency toward hydrogenation of various unsaturated molecules will be developed. The methods and results of the current project are expected to provide substantial theoretical and experimental support for technology innovation and competitiveness enhancement of petrochemical and pharmaceutical industries of our nation.

英文关键词： Catalytic machanism;Selective hydrogenation;Transition metal carbides;Transition metal oxides;Hydrogen spillover