Engineering Atom‐Scale Cascade Catalysis via Multi‐Active Site Collaboration for Ampere‐Level CO 2 Electroreduction to C 2+ Products

作者：Cheng‐Hao Jin, Lin Yue, Yanan Wang, Yanan Wang, Jingbo Shi, Li Ren, Yijiang Liu, Zongye Yue, Kunyue Leng, Yafei Zhao, Yi Wang, Yi Wang, Xiao Han, Yunteng Qu, Jinbo Bai · 发表于：Advanced Materials · 年份：2025 · DOI：10.1002/adma.202412658 · 被引用次数：42 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Electrocatalysts for Energy Conversion

Abstract Electrochemical reduction of CO 2 to value‐added multicarbon (C 2+ ) productions offers an attractive route for renewable energy storage and CO 2 utilization, but it remains challenging to achieve high C 2+ selectivity at industrial‐level current density. Herein, a Mo 1 Cu single‐atom alloy (SAA) catalyst is reported that displays a remarkable C 2+ Faradaic efficiency of 86.4% under 0.80 A cm −2 . Furthermore, the C 2+ partial current density over Mo 1 Cu reaches 1.33 A cm −2 with a Faradaic efficiency surpasses 74.3%. The combination of operando spectroscopy and density functional theory (DFT) indicates the as‐prepared Mo 1 Cu SAA catalyst enables atom‐scale cascade catalysis via multi‐active site collaboration. The introduced Mo sites promote the H 2 O dissociation to fabricate active * H, meanwhile, the Cu sites (Cu 0 ) far from Mo atom are active sites for the CO 2 activation toward CO. Further, CO and * H are captured by the adjacent Cu sites (Cu &+ ) near Mo atom, accelerating CO conversion and C─C coupling process. Our findings benefit the design of tandem electrocatalysts at atomic scale for transforming CO 2 to multicarbon products under a high conversion rate.