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

This is the authors' abstract. We don't add key points for this paper.

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.