二氧化碳加氢合成甲酸纳米金催化剂的构建

项目名称： 二氧化碳加氢合成甲酸纳米金催化剂的构建

项目编号： No.21676045

项目类型： 面上项目

立项/批准年度： 2017

项目学科： 有机化学

项目作者： 王新葵

作者单位： 大连理工大学

项目金额： 30万元

中文摘要： 开发二氧化碳加氢合成甲酸多相催化剂新体系是一个具有挑战性的课题。对载体表面进行胺基功能化有望为这一问题的解决提供一种新思路。本项目旨在前期开发的席夫碱功能化的纳米金催化剂可以高效分解高浓度甲酸及其催化二氧化碳加氢合成甲酸的基础上，进一步研究催化剂表面胺基、金属粒子大小、组成、金属与载体之间的相互作用等因素对二氧化碳加氢合成甲酸反应性能的影响规律；利用原位红外技术和密度泛函计算研究二氧化碳在催化剂表面的吸附活化历程、反应中间物种的性质与催化活性之间的内在联系；阐明催化剂表面胺基基团与纳米金粒子在催化二氧化碳加氢合成甲酸中的协同作用机制，探讨二氧化碳的活化机理。本项目的实施为深入认识二氧化碳的活化机理、二氧化碳加氢合成甲酸多相催化体系的设计制备提供参考。

中文关键词： 二氧化碳；纳米金；甲酸；催化加氢

英文摘要： Developing new heterogeneous catalysts for carbon dioxide hydrogenation to formic acid is a challenging subject, to which the functionalization of the catalyst support surface by amine groups might be a solution. Based on our previously developed Schiff base-functionalized nano-gold catalysts which proved efficient towards the dehydrogenation of formic acid and carbon dioxide hydrogenation to formic acid, this project will further study the impacts of the surface amine groups of the catalyst, the particle size, the composition of the metal component, the interaction between metal and support on the performance of the catalysts in carbon dioxide hydrogenation to formic acid. The in-situ FTIR and DFT will be utilized to investigate the adsorption/activation of carbon dioxide on the catalyst surface, and the relationship between the properties of the reaction intermediates and the catalytic activity of the catalyst. This project will clarify the synergism between the surface amine groups and gold in carbon dioxide hydrogenation to formic acid, and discuss the activation mechanism of carbon dioxide. The research results will provide instructions for the in-depth understanding of the activation mechanism of carbon dioxide, and for the design of highly efficient heterogeneous catalysts for carbon dioxide hydrogenation to formic acid.

英文关键词： carbon dioxide;nano-gold ;formic acid;catalytic hydrogenation