Engineering Atom-Scale Cascade Catalysis via Multi-Active Site Collaboration for Ampere-Level CO Electroreduction to C Products.

Electrochemical reduction of CO to value-added multicarbon (C) productions offers an attractive route for renewable energy storage and CO utilization, but it remains challenging to achieve high C selectivity at industrial-level current density. Herein, a MoCu single-atom alloy (SAA) catalyst is reported that displays a remarkable C Faradaic efficiency of 86.4% under 0.80 A cm. Furthermore, the C partial current density over MoCu reaches 1.33 A cm with a Faradaic efficiency surpasses 74.3%. The combination of operando spectroscopy and density functional theory (DFT) indicates the as-prepared MoCu SAA catalyst enables atom-scale cascade catalysis via multi-active site collaboration. The introduced Mo sites promote the HO dissociation to fabricate active H, meanwhile, the Cu sites (Cu) far from Mo atom are active sites for the CO 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 to multicarbon products under a high conversion rate.