堆垛层错型催化剂的可控构筑及流动相电解池电催化CO2还原研究

电催化CO2还原生成高附加的化学品是实现CO2减排和资源化利用的前沿技术，该技术的进一步发展强烈依赖于高性能电催化剂的可控构筑及其新型稳定的气体扩散电极的开发。本项目拟采用物理激光脉冲消融法可控地构筑堆垛层错型催化剂，通过堆垛层错的密度来精确调控催化剂表面原子结构和晶格应力，从而提升催化剂对CO2的吸附性能，降低CO2活化的过电位，提高电催化CO2还原产物的选择性和反应活性，并通过多物理场仿真优化气体扩散电极的结构，实现堆垛层错型催化剂在流动相电解池中高效地电催化CO2还原。系统探究堆垛层错型催化剂对CO2吸附性能的影响规律；阐明催化剂表面原子结构和晶格应力与电催化CO2还原性能之间的构效关系；结合理论计算和原位表征技术，揭示堆垛层错型催化剂电催化CO2还原的反应机理。该项目的实施可为新型催化剂的开发提供理论基础和实验依据，对推动CO2的减排和资源化利用具有重要意义。

Electrocatalytic CO2 reduction into valuable chemicals is a cutting-edge technology for mitigating CO2 emissions and CO2 utilizations. However, the further development of this advanced technology highly depends on the electrocatalysts with excellent catalytic performance and stable gas diffusion electrodes. In this project, it is proposed to controllably construct stacking fault catalysts by the physical laser pulse ablation strategy. To enhance CO2 adsorption ability, lower the CO2 activation overpotentials and improve the selectivity of products and reaction activity, the surface structure and strain of the catalyst are tuned by the stacking fault density. Optimized the structure of gas diffusion electrodes by the multi-physics field simulation. It is expected that the gas diffusion electrodes with stacking fault catalysts can effectively boost electrocatalytic CO2 reduction activity in the flow cell. The influences of stacking fault catalysts on the adsorption activity of CO2 will be explored in detail. Besides, the structure-activity relationship between the surface atomic structure/strain and electrocatalytic CO2 reduction performance will be also studied. Afterward, the DFT theoretical calculation and some in-situ characterizations will be employed to study the mechanism of the electrocatalytic CO2 reduction reaction from stacking fault catalysts. This project can provide experimental basics and theoretical guidance for the development of electrocatalysts, and promote CO2 emission cuts and CO2 utilization.