LAUSR

Despite its importance for the establishment of a carbon‐neutral society, the electrochemical reduction of CO2 to value‐added products has not been commercialized yet because of its sluggish kinetics and low selectivity. The present work reports the fabrication of a low‐crystalline trimetallic (AuCuIn) CO2 electroreduction catalyst and demonstrates its high performance in a gaseous CO2 electrolyzer. The high Faradaic efficiency (FE) of CO formation observed at a low overpotential in a half‐cell test is ascribed to the controlled crystallinity and composition of this catalyst as well as to its faster charge transfer, downshifted d‐band center, and low oxophilicity. The gaseous CO2 electrolyzer with the optimal catalyst as the cathode exhibits superior cell performance with a high CO FE and production rate, outperforming state‐of‐the‐art analogs. Thus, the obtained results pave the way to the commercialization of CO2 electrolyzers and promote the establishment of a greener society.