Tian Meng, Wu Shanshan, Hu Yang, Mu Zhaori, Li Zhi, Hou Yichao, Xi Pinxian, Yan Chun-Hua
State Key Laboratory of Applied Organic Chemistry, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China.
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering Peking University, Beijing 100871, China.
Nanoscale. 2023 Mar 2;15(9):4477-4487. doi: 10.1039/d2nr06638f.
Electrocatalytic reduction of CO to formate is considered as a promising method to achieve carbon neutrality, and the introduction of heteroatoms is an effective strategy to improve the catalytic activity and selectivity of catalysts. However, the structural reconstruction behavior of catalysts driven by voltage is usually ignored. Therefore, we used Cu/BiS as a model to reveal the dynamic reduction process in different atmospheric environments. The catalyst showed an outstanding faradaic efficiency of 94% for formate and a long-term stability of 100 h, and exhibited a high current density of 280 mA cm in a flow cell. The experimental results and theoretical calculations show that the introduction of copper enhances the adsorption of CO, accelerates the charge transfer and reduces the formation barrier of *OCHO, thus promoting the formation of formate. This work draws attention to the effects of saturated gases in the electrolyte during structural evolution and provides a possibility for designing catalysts with high catalytic activity.
将CO电催化还原为甲酸盐被认为是实现碳中和的一种有前景的方法，引入杂原子是提高催化剂催化活性和选择性的有效策略。然而，通常忽略了由电压驱动的催化剂结构重构行为。因此，我们以Cu/BiS为模型来揭示不同大气环境下的动态还原过程。该催化剂对甲酸盐显示出94%的出色法拉第效率和100小时的长期稳定性，并且在流动池中表现出280 mA cm的高电流密度。实验结果和理论计算表明，铜的引入增强了CO的吸附，加速了电荷转移并降低了*OCHO的形成势垒，从而促进了甲酸盐的形成。这项工作引起了人们对结构演化过程中电解质中饱和气体影响的关注，并为设计具有高催化活性的催化剂提供了可能性。
