多孔Cu/M（M=Ag、Au）双活性位金属催化剂的构建及电催化CO2还原制C2产物的研究

电催化CO2还原制高附加值化学品，因其在环境和能源领域极具前景而备受关注。然而，此项研究仍面临效率低、稳定性差和C2产物选择性低等问题，其原因在催化剂的可控合成、活性位的多尺度精准构筑和原位反应过程研究等方面缺乏有效方法。本项目拟构筑多孔Cu/M（M=Ag、Au）双活性位金属催化剂，利用多孔结构和双活性位的协同作用增效电催化CO2还原制C2产物。系统考察催化剂的孔结构、M种类、M比例、M空间分布等对C2产物选择性的影响。在此基础上，利用原位表征技术探究CO2在催化剂表界面的吸附、反应中间体CO在催化活性位的生成、迁移机制，并结合理论计算进行验证、解释和分析，从分子/原子水平阐明孔结构和双活性位对电催化CO2还原制C2产物的协同增效机制。本项目顺利实施为CO2减排和高效资源化转化提供理论依据和技术支持。

Electrocatalytic CO2 reduction into the high value-added chemicals has attracted considerable attention because of its promising application in energy and environmental fields. However, this study still has the shortages of low efficiency, poor stability and low selectivity of C2 products, possibly due to the lack of effective method in controlled synthesis of catalysts, accurate construction of multi-scale active sites, and in-situ monitoring during the reaction process. This project intends to construct the porous Cu/M (M=Ag、Au) metallic catalyst with bi-active sites and study the synergistic effect of porous structure and bi-active sites for enhancing the selectivity of the C2 products. The effect of parameters such as the porous structure、M species、M molar ratio and the spatial distribution on the selectivity of C2 products was systematic investigated in this project. Based on above study, the in-situ techniques are further utilized to study the behavior of CO2 adsorption, and the formation and migration mechanism of intermediate CO on catalytic active site. Finally, the synergistic effect could be explained from the molecular/atomic level based on the in-situ technical study and the theoretical calculation. This project provides important theoretical and technical support for study of the CO2 reduction and the efficient utilization of CO2 resources.