Chen Zhipeng, Zhao Yusi, Liu Gen, Zhang Hongna, Yan Yan, Ke Qingping, Liu Mingkai, Liu Licheng, Lin Zhiqun
School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma'anshan 243032, P. R. China.
College of Chemistry & Chemical Engineering, Ocean University of China, Qingdao 266100, P. R. China.
Nano Lett. 2025 Apr 23;25(16):6771-6779. doi: 10.1021/acs.nanolett.5c01205. Epub 2025 Apr 10.
The predominant product of CO electroreduction (COER) is often acetate, with the Faradaic efficiency (FE) for ethanol usually falling below 50%. Herein, we propose a unique strategy to enhance product selectivity in COER, shifting it from acetate predominance toward ethanol generation via alloying atomic manganese (Mn) atoms with a face-centered cubic (FCC) copper (Cu) catalyst. By optimizing the atomic ratio of Mn to Cu, we observe an impressive enhancement of 8.8-fold for the ethanol-to-acetate FE ratio in the optimal MnCu alloy compared to unalloyed FCC-phase Cu. MnCu demonstrates a remarkable ethanol FE of nearly 70% at a high current density of 600 mA cm in a membrane electrode assembly electrolyzer. Further theoretical analysis reveals that atomically dispersed Mn atoms generate synergistic active sites and modulate the adsorption strength of critical intermediates relevant to ethanol synthesis, thereby facilitating the transition from the acetate pathway to the ethanol pathway.
一氧化碳电还原（COER）的主要产物通常是乙酸盐，乙醇的法拉第效率（FE）通常低于50%。在此，我们提出了一种独特的策略来提高COER中的产物选择性，通过将原子锰（Mn）与面心立方（FCC）铜（Cu）催化剂合金化，使其从以乙酸盐为主转变为生成乙醇。通过优化Mn与Cu的原子比，我们观察到，与未合金化的FCC相Cu相比，最佳MnCu合金中乙醇与乙酸盐的FE比提高了8.8倍，令人印象深刻。在膜电极组件电解槽中，MnCu在600 mA cm的高电流密度下表现出近70%的显著乙醇FE。进一步的理论分析表明，原子分散的Mn原子产生协同活性位点，并调节与乙醇合成相关的关键中间体的吸附强度，从而促进从乙酸盐途径向乙醇途径的转变。
