Guo Xinhui, Liu Tianfu, Song Yanpeng, Li Rongtan, Wei Pengfei, Liao Ziqi, Wu Zichao, Gao Dunfeng, Fu Qiang, Wang Guoxiong, Bao Xinhe
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2025 Jul 7;64(28):e202507062. doi: 10.1002/anie.202507062. Epub 2025 May 19.
Electrochemical carbon monoxide reduction reaction (CORR) to produce multicarbon (C) oxygenates using renewable electricity is a promising carbon utilization pathway. However, the performance of this process suffers from low C oxygenates selectivity and insufficient current density. Here, we employed a Cu-Ag bimetallic strategy to enhance the selectivity of C oxygenates from CORR in alkaline membrane electrode assembly electrolyzer at ampere-level current densities. The Cu-Ag catalysts prepared by magnetron sputtering feature atomically dispersed Cu-Ag sites on the catalyst surface, which are key to promoting the formation of C oxygenates. Increasing Ag content favors C oxygenates formation while inhibiting ethylene production. The optimized CuAg catalyst achieved Faradaic efficiency of 71.4% for C oxygenates at 2.5 A cm. In situ spectroscopy and density functional theory calculations revealed that atomically dispersed Cu-Ag sites on the catalyst surface promote the dissociation of *COCOH to *CCO, thus favoring C oxygenates formation.
利用可再生电力通过电化学一氧化碳还原反应（CORR）生产多碳（C）含氧化合物是一条很有前景的碳利用途径。然而，该过程的性能受到低C含氧化合物选择性和电流密度不足的影响。在此，我们采用铜-银双金属策略，以提高碱性膜电极组件电解槽中安培级电流密度下CORR生成C含氧化合物的选择性。通过磁控溅射制备的铜-银催化剂在催化剂表面具有原子分散的铜-银位点，这是促进C含氧化合物形成的关键。增加银含量有利于C含氧化合物的形成，同时抑制乙烯的产生。优化后的铜银催化剂在2.5 A/cm²时对C含氧化合物的法拉第效率达到71.4%。原位光谱和密度泛函理论计算表明，催化剂表面原子分散的铜-银位点促进COCOH解离为CCO，从而有利于C含氧化合物的形成。
