混合电解质中Cu基多元金属电催化CO2高效还原制备C2+化合物研究

设计高效催化体系，电催化CO2转化制备C2及以上（C2+）化合物是重要前沿方向，但有诸多难题有待解决。本项目针对电催化CO2转化为C2+产物的还原反应，设计合成杂原子（N、N/S、N/P/F等）掺杂氧化石墨烯担载Cu基多元金属（Cu-Sm、Cu-Ir、Cu-Ni-Rh等）催化材料，设计和筛选不同离子液体、离子液体/水、离子液体/有机溶剂、离子液体/有机溶剂/水等电解质，构建高效电催化材料-电解质体系。系统研究催化材料组成与结构、电解质组成与结构、催化材料-电解质界面性质、电解质与CO2相互作用对反应电流效率、产物选择性的影响，优化反应条件。将理论与实验相结合，研究反应过程中形成C2+产物的关键中间体、催化活性中心和C-C偶联机制、催化材料构效关系、催化材料中各组分之间协同作用、反应机理、电解质与催化材料之间的匹配和协同效应规律和机理，为CO2高效绿色转化为高值化学品和燃料奠定科学基础。

The design of highly efficient catalytic systems to facilitate electrocatalytic conversion of CO2 into C2+ compounds（including C2）is an important frontier research topic. However, there are a number of difficult issues that need to be addressed. To promote electroreduction of CO2 to produce C2+ products, heteroatom（N, N/S, N/P/F, etc.）-doped graphene oxide supported Cu-based multimetal（Cu-Sm, Cu-Ir, Cu-Ni-Rh, etc.）electrocatalytic materials will be designed and synthesized in the present research proposal. Meanwhile, different electrolytes including a series of ionic liquids（ILs）, IL/water, ILs/organic solvent, IL/organic solvent/water will be designed and screened. Highly efficient electrocatalytic material-electrolyte systems will be created. The effects of electrocatalytic material’s composition and structure, electrolyte’s composition and structure, properties of electrocatalytic material-electrolyte interface, interaction between electrolyte and CO2 molecule on both reaction current efficiency and product selectivity will be systematically explored. Reaction conditions will be optimized. Theory calculations and experiments will be combined to study key C2+ product intermediates, catalytic active centers, and C-C coupling mechanisms. Structure-activity relationship of electrocatalytic materials, synergistic effects among different components of electrocatalytic materials, reaction mechanisms as well as matching and synergistic effects between electrolytes and catalytic materials will also be investigated. This project will provide scientific foundation for efficient and green conversion of CO2 into high-value added products and fuels.