Wang Min, Fang Minghui, Liu Yingxuan, Chen Chunjun, Zhang Yichi, Jia Shuaiqiang, Wu Haihong, He Mingyuan, Han Buxing
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.
Institute of Eco-Chongming, 20 Cuiniao Road, Chenjia Town, Chongming District, Shanghai 202162, China.
J Am Chem Soc. 2025 May 14;147(19):16450-16458. doi: 10.1021/jacs.5c03057. Epub 2025 May 2.
Electrochemical CO reduction reaction (CORR) to multicarbon (C) products holds immense significance in promoting a closed carbon cycle and solving global energy problems, but it faces challenges of unsatisfactory selectivity. In this work, we constructed an Ag single-atom alloy cascade catalyst (AgCu-SAA) using an epoxide gelation approach, which enhanced the utilization efficiency of the CO intermediate through an inter-migration pathway. As a result, the C products' Faradaic efficiency (FE) of 83.4% was achieved at a current density of 900 mA cm. Moreover, the FE of the C products remained as high as 74.8% even at a high current density of 1100 mA cm. In situ Raman spectra and density functional theory (DFT) calculations reveal that CO is first converted to CO over the single-atom Ag site. Subsequently, the generated CO is directly transferred to the adjacent Cu site rather than desorbing into the electrolyte. This process avoids the inefficient migration of CO inter-mediates, thereby enhancing the selectivity for the formation of C products.
电化学将一氧化碳还原反应（CORR）转化为多碳（C）产物在促进封闭碳循环和解决全球能源问题方面具有重大意义，但面临选择性不尽人意的挑战。在这项工作中，我们采用环氧化物凝胶法构建了一种银单原子合金级联催化剂（AgCu-SAA），其通过一种相互迁移途径提高了CO中间体的利用效率。结果，在900 mA cm的电流密度下实现了83.4%的C产物法拉第效率（FE）。此外，即使在1100 mA cm的高电流密度下，C产物的FE仍高达74.8%。原位拉曼光谱和密度泛函理论（DFT）计算表明，CO首先在单原子银位点上转化为CO。随后，生成的CO直接转移到相邻的铜位点，而不是解吸到电解液中。这一过程避免了CO中间体的低效迁移，从而提高了形成C产物的选择性。
