methanol synthesis

electrochemical reduction

catalytic activity

catalytic performance

reduction reaction

faradaic efficiency

activity selectivity

Angewandte Chemie

Single atom catalysts (SACs) have been widely studied in the field of CO 2 electroreduction, but industrial‐level current density and near‐unity product selectivity are still difficult to achieve. Herein, a diatomic site catalysts (DASCs) consisting of Co‐Cu hetero‐diatomic pairs is synthesized. The CoCu DASC exhibits excellent selectivity with the maximum CO Faradaic efficiency of 99.1 %. The CO selectivity can maintain above 95 % over a wide current density range from 100 mA cm −2 to 500 mA cm −2 . The maximum CO partial current density can reach to 483 mA cm −2 in flow cell, far exceed industrial‐level current density requirements (&gt;200 mA cm −2 ). Theoretical calculation reveals that the synergistic catalysis of the Co‐Cu bimetallic sites reduce the activation energy and promote the formation of intermediate *COOH. This work shows that the introduction of another metal atom into SACs can significantly affect the electronic structure and then enhance the catalytic activity of SACs.

Design of Co-Cu Diatomic Site Catalysts for High-efficiency Synergistic CO2 Electroreduction at Industrial-level Current Density.