Lewis Acid Site-Promoted Single-Atomic Cu Catalyzes Electrochemical CO Methanation.

Developing an efficient catalyst for the electrocatalytic CO reduction reaction (CORR) is highly desired because of environmental and energy issues. Herein, we report a single-atomic-site Cu catalyst supported by a Lewis acid for electrocatalytic CO reduction to CH. Theoretical calculations suggested that Lewis acid sites in metal oxides (e.g., AlO, CrO) can regulate the electronic structure of Cu atoms by optimizing intermediate absorption to promote CO methanation. Based on these theoretical results, ultrathin porous AlO with enriched Lewis acid sites was explored as an anchor for Cu single atoms; this modification achieved a faradaic efficiency (FE) of 62% at -1.2 V (vs RHE) with a corresponding current density of 153.0 mA cm for CH formation. This work demonstrates an effective strategy for tailoring the electronic structure of Cu single atoms for the highly efficient reduction of CO into CH.