CO2电催化还原反应中的催化剂表界面精细原子调控

Electrochemical reduction reaction of CO2 (CO2RR) is an effective approach to CO2 conversion, which could help to solve the current issues on energy and environment, and therefore is of paramount social values. During the process of electrochemical reduction, the adsorption, activation and desorption of CO2 molecules on the surface/interface of catalysts are the key factors that dictate the performance. The research focus of this project is to precisely manipulate the nanocatalyst interface on the atomic level, to rationally design and prepare high-performance nanocatalysts for CO2RR. The applicant plans to center on the activity and selectivity of aqueous-phase CO2RR, to select metallic and metal/oxide nanomaterials as the target systems. The applicant expects to make breakthroughs in the atomic-level surface manipulation of nanocatalysts, to construct specific catalytic facets by design and controlled synthesis, to conduct studies on the CO2RR catalytic performances, to unveil the reaction mechanisms via in-situ characterizations and theoretical calculations, and to promote the development and applications of high-performance CO2RR nanocatalysts.

CO2电化学还原反应（CO2RR）是一种有效的CO2转化途径，有助于解决当下环境和能源问题，具有重要的社会和经济价值。在电化学还原过程中，CO2分子在催化材料表界面的吸附、活化和脱附，是影响其性能的关键因素。对催化剂表界面进行原子级精细调控，理性设计并制备出高效的CO2RR催化剂是本项目研究的重点。申请人拟围绕水体系CO2RR的活性和选择性问题，以金属和金属/氧化物纳米材料为研究对象，选择表界面精细原子调控为材料制备的突破点，通过设计和精准的合成，构建特定催化表界面，开展CO2RR催化性能研究，并结合原位表征和理论计算进行反应机理研究，推动高效CO2RR纳米催化剂的发展和应用。

本项目对催化材料表界面进行精细调控，发展了若干用于CO2电催化还原的催化剂，实现了CO2电还原性能的优化，并探索了反应机理，顺利完成研究目标。受本项目资助，发表标注论文36 篇，其中包括Nat. Chem. 1篇、Chem 1篇、Nat. Commun. 4篇、J. Am. Chem. Soc. 2篇、Angew. Chem. Int. Ed. 2篇、Adv. Mater. 3篇、Energy Environ. Sci. 1篇、Chem. Sci. 3篇等。受本项目资助培养的已毕业博士生7人、出站博士后7人。