二元金属团簇/石墨炔复合体系电催化还原N2的理论研究

为了解决N2还原NH3过程中面临的一个由氮活化和析氢竞争反应组成的困境，设计出具有高活性、高选择性且催化活性可以受应力调控的催化材料是目前需要解决的关键科学问题。本项目采用第一性原理对二元金属团簇/石墨炔（MxM’3-x/GDY）复合体系展开系统而深入地研究。探寻复合体系的结构和催化性质随团簇元素组分、配比的变化规律，分析复合体系内团簇与表面间复杂的相互作用，探讨应力对复合体系的结构和催化性质的调控，深层次理解复合体系内局域电子之间以及局域电子与离域电子之间的耦合机制，揭示影响催化性质的物理根源以及调控催化性质的途径和规律。本项目的顺利实施与成功将从理论上为设计高活性、高选择性的N2还原催化材料提供新思路和新途径。

To solve the dilemma of nitrogen activation and competitive reaction of hydrogen evolution, it is a key scientific issue to design the catalytic materials with high activity, high selectivtiy and facilely manipulated catalytic properties by strain. In this project, we will investigate the complex system of binary metal clusters/graphdiyne (MxM’3-x/GDY) using first principle calculation. We will search for the variations of structures and catalytic properties for the complex system with the changes of cluster size, component, proportion, and analyze the complicated interaction between cluster and surface, meanwhile discuss the response of the structure and catalytcic property of complex system to external strain, and reveal the physical essence of the impact factors for catalytic properties and methods and rules regulating the catalytic properties of clusters, and understand deeply coupling mechanism of the homogeneous atoms and heterogeneous atoms. The successful implementation of the project will provide theoretically new ideas and new ways in high activkity and high selectivity catalytic materials for nitrogen reduction.