本项目针对指南中碳基材料研究以及煤炭生产中的三废利用和碳减排，拟结合氮掺杂石墨烯（NG）在CO2加氢反应中的应用前景，以钌的配合物[Ru]为活性中心，利用重氮化反应将其共价链接至NG表面，构建新型、高效碳基材料[Ru]/NG，用于催化CO2加氢制甲醇。拟通过调节重氮化反应条件、金属配合物的配体以及取代基，从而从原子水平、分子尺度精准调控催化剂表界面的结构。拟采用掺杂氮物种的pKa、氮物种‒CO2结合的平衡常数、同位素示踪、电化学等手段研究催化剂表界面上反应物的吸附活化以及活性物种之间的反应机制。拟揭示NG载体对CO2的捕集和固定机制，阐明CO2在催化剂表界面的选择活化和定向转化机理。拟发展通过催化材料表界面结构的设计和调控以提高其催化特性的新方法。研究成果将为碳基催化材料结构的精准设计和调控提供一种新思路，为CO2高值转化与规模化利用提供理论支持，因而具有重要基础研究价值和重大社会意义。

This project is aimed at the funding guideline on the study of fundamental research of carbon-based materials, comprehensive utilization of "three wastes" and carbon emission reduction during coal production. By combinating a wide application prospect of nitrogen-doped graphene (NG) in CO2 hydrogenation, novel and efficient catalysts ([Ru]/NG) are prepared by covalently grafting Ru complexes to NG by diazotization reaction in this research. The accurate tuning of atomic and electronic structures on local areas of catalyst surface and interface can be realized on atomic and molecular levels by diazotization conditions, ligands and substituent groups of Ru complexes. The adsorption and activation of reactants and reaction mechanism of active species on the catalyst surface and interface are investigated by pKa of nitrogen-doped species, equilibrium constant of nitrogen species and CO2, isotope tracer and electrochemistry. The goal of this research is to realize the the principle of capture and fixation of NG support to CO2, to understand the mechanism of selective activation and directional conversion of CO2 on the catalyst surface and interface, and to develop new methods by which the catalytic performance is improved by the structure tuning of catalyst surface and interface. The research will provide a new insight into the accurate design and construction of atomic and electronic structures on local areas of catalyst and promote the understanding of reaction rules on the catalyst surface and interface for high value transformation and scale utilization of CO2.