Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene

作者：Yanteng Xiao, Fuqing Yu, Chenfeng Xia, Deyu Zhu, Jiwen Chen, Nengji Liu, Yuye Zhao, Ruijuan Qi, Wei Guo, Bo You, Tao Yao, Yuanjie Pang, Ziyun Wang, Hongming Wang, Fei Song, Bao Yu Xia · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c02896 · 被引用次数：118 · 研究领域：CO2 Reduction Techniques and Catalysts、Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science

The electrocatalytic conversion of carbon dioxide (CO 2 ) to ethylene (C 2 H 4 ) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified a praseodymium (Pr) single-atom alloy embedded in a copper (Cu) catalyst (Pr@Cu) that exhibits superior CO 2 activation and a remarkably low energy barrier for asymmetric *CO–*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves a C 2 H 4 Faradaic efficiency (FE) of 64.2% at −1.6 V versus the reversible hydrogen electrode (RHE) under a high current density of 1200 mA cm –2 in the CO 2 reduction reaction (CO 2 RR). Furthermore, when integrated into a 100 cm 2 membrane electrode assembly (MEA) electrolyzer, Pr@Cu-2 demonstrates robust performance, maintaining a continuous C 2 H 4 production rate of 21.3 mL min –1 at 20 A for over 200 h. This work provides fundamental insights into the role of Pr single-atom alloys in the CO 2 RR and highlights their potential for scalable C 2 H 4 electrosynthesis.