Feng Zemin, Hu Chenghong, Tang Huangcong, Shen Kui, Chen Liyu, Li Yingwei
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology Guangzhou 510640 China
Chem Sci. 2025 Apr 21. doi: 10.1039/d4sc07772e.
Single-atomic Cu catalysts show promise for the electrochemical CO reduction (CORR) to acetate, but their efficiency is limited by the difficulty in generating the CO intermediate needed for C-C coupling. While co-catalysts can enhance CO generation, weak interaction between co-catalytic and single-atom Cu sites hinders CO spillover, resulting in low acetate yield. Herein, we design atomic Cu-Ag pairs to enhance CO generation and facilitate CO spillover from Ag to Cu in the CORR to enhance acetate production. The Cu-Ag/NC catalyst shows a high faradaic efficiency of 50% for acetate and 72% for C products at -0.5 V a reversible hydrogen electrode, significantly outperforming single-atomic Cu catalysts. Theoretical calculations and characterization demonstrate that the Cu-Ag bonding can facilitate the *CO spillover from Ag to Cu sites, while the electronic modification of Cu by Ag accelerates the subsequent formation of acetate on Cu sites.
单原子铜催化剂在电化学将一氧化碳还原为乙酸盐方面展现出前景，但其效率受到生成碳-碳偶联所需一氧化碳中间体困难的限制。虽然助催化剂可以增强一氧化碳的生成，但助催化位点与单原子铜位点之间的弱相互作用阻碍了一氧化碳的溢流，导致乙酸盐产率较低。在此，我们设计了原子级的铜-银对，以增强一氧化碳的生成，并在电化学一氧化碳还原反应中促进一氧化碳从银溢流到铜，从而提高乙酸盐的产量。在相对于可逆氢电极-0.5 V的电位下，铜-银/氮碳催化剂对乙酸盐的法拉第效率高达50%，对含碳产物的法拉第效率为72%，显著优于单原子铜催化剂。理论计算和表征表明，铜-银键合可以促进*CO从银位点溢流到铜位点，而银对铜的电子修饰加速了随后在铜位点上乙酸盐的形成。
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