双核型单分子异质结催化剂的定制及其CO2还原产物的电化学调控

实现电催化CO2有效转化为高附加值的化学原料和清洁燃料对解决能源和环境危机具有重要的战略意义，而构建高效稳定的电催化剂是实现这一目标的核心。近年来，虽然电催化CO2还原制高级产物取得了一定的进展，但受限于催化剂活性位点单一、对催化机制的理解尚不深入等原因，其高级产物的选择性依然不理想。本项目拟设计合成结构明确、具有共轭平面的双核金属配合物，实现金属配位原子和电子结构的精准调控。继而以功能化碳基材料为锚定载体，通过分子尺度构建策略制备一系列具有高表面活性密度的双核型单分子异质结催化材料。基于活性位点的灵活设计和界面驱动的局域协同，探索电催化CO2还原产物的高效调控和模块化制备，深入研究配位原子组成、局域电子结构和催化性能之间的科学关系，继以筛选出具有商业价值的电催化CO2还原催化剂。本项目的开展不仅为单分子异质结催化剂的可控制备提供重要参考，而且为CO2高效转化的深入研究和广泛应用奠定基础。

Efficiently electrocatalytic conversion CO2 to high-value-added chemical feedstocks and clean fuels has important strategic significance in solving energy and environmental crisis. The development of efficient and stable electrocatalysts is the key to achieve this aim. Although some developments on electrocatalytic CO2 to advanced products were made recently, it is still not adequate to deeply understand the catalysis mechanism and high-selectively obtain the advanced products because of lack of versatile catalysts. In this project, we propose to design and synthesize a series of binuclear metal complexes with well-defined structure. Then they will be converted into binuclear single-molecular heterojunction catalysts with highly surface activity density through controllable molecular scale construction strategy. Based on the flexible design and local synergy of active sites, the efficient regulation and modular preparation of electrocatalytic CO2 reduction products were explored, followed by screening of electrocatalysts with commercial value. The development of this project is not only expected to provide valuable references for the controlled synthesis of single-molecular heterojunction-type catalysts, but also expected to promote the in-depth study and wide application of efficient CO2 conversion.