Interfacial Engineering of Ag/C Catalysts for Practical Electrochemical CO₂ Reduction to CO

Abstract

Electrochemical CO2 reduction to value‐added chemicals by renewable energy sources is a promising way to implement the artificial carbon cycle. During the reaction, especially at high current densities for practical applications, the complex interaction between the key intermediates and the active sites would affect the selectivity, while the reconfiguration of electrocatalysts could restrict the stability. This paper describes the fabrication of Ag/C catalysts with a well‐engineered interfacial structure, in which Ag nanoparticles are partially encapsulated by C supports. The obtained electrocatalyst exhibits CO Faradaic efficiencies (FEs) of over 90% at current densities even as high as 1.1 A/cm2. The strong interfacial interaction between Ag and C leads to highly localized electron density that promotes the rate‐determining electron transfer step by enhancing the adsorption and the stabilization of the key *COO‒ intermediate. In addition, the partially encapsulated structure prevents the reconfiguration of Ag during the reaction. Stable performance for over 600 h at 500 mA/cm2 is achieved with CO FE maintaining over 95%, which is among the best stability with such a high selectivity and current density. This work provides a novel catalyst design showing the potential for the practical application of electrochemical reduction of CO2.