有机小分子可再生氢能源：过渡金属多功能仿生催化机制的理论研究

项目名称： 有机小分子可再生氢能源：过渡金属多功能仿生催化机制的理论研究

项目编号： No.21473261

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： 柯卓锋

作者单位： 中山大学

项目金额： 80万元

中文摘要： 源于生物启发的过渡金属多功能仿生催化，可以通过有机小分子制氢储氢，制备可再生液体氢燃料，在应对能源危机方面有着重要的科学意义和广阔的应用前景。针对目前研究面临的多功能催化剂结构和反应机理复杂，常规实验观察和表征认识有限的现状，本项目将从基础理论角度出发，通过理论与计算化学研究，阐明过渡金属多功能仿生催化有机分子制氢储氢的机理，解释Lewis酸/碱功能团的辅助作用机制，以及影响催化活性的关键步骤，揭示关键活性中间体及其催化活性的影响要素。通过系统研究深入认识仿生多功能过渡金属催化剂的结构-活性-机理之间的规律，为实现多功能仿生催化策略，设计新颖高效的有机小分子制氢储氢过渡金属催化体系提供理论指导和思路

中文关键词： 密度泛函计算；催化机理；电子结构；仿生催化；氢能源

英文摘要： Bio-inspired multi-functional transition metal (TM) catalysis is a promising way to catalyze the storage and release of hydrogen via small organic molecules, which is of fundamental importance and has intriguing potential in fuel applications with regard to the energy crisis. However, the experimental study of bio-inspired multi-functional TM catalyzed storage and release of hydrogen via small organic molecules is still at the infant stage, facing with the difficulties in understanding the active site structure and reaction mechanism. We plan to perform theoretical and computational study to disclose the catalytic mechanism for this kind of bio-inspired multi-functional TM systems, especially how the Lewis acid/base functional groups involve in the catalyticcycle. Our study will help to reveal the key steps of the catalytic cycles, the important active intermediates, and the structural factors that play important role in the activity. Base on the understanding of the structure-activity-mechanism, this study will provide insights and guidelines for the design and development of novel and efficient bio-inspired multi-functional TM catalysts for the storage and release of hydrogen via small organic molecules.

英文关键词： DFT calculation;catalytic mechanism;electronic structure;bio-inspired catalysis;hydrogen energy