MXene‐Regulated Metal‐Oxide Interfaces with Modified Intermediate Configurations Realizing Nearly 100% CO2 Electrocatalytic Conversion

Abstract Electrocatalytic CO 2 reduction via renewable electricity provides a sustainable way to produce valued chemicals, while it suffers from low activity and selectivity. Herein, we constructed a novel catalyst with unique Ti 3 C 2 T x MXene‐regulated Ag−ZnO interfaces, undercoordinated surface sites, as well as mesoporous nanostructures. The designed Ag−ZnO/Ti 3 C 2 T x catalyst achieves an outstanding CO 2 conversion performance of a nearly 100% CO Faraday efficiency with high partial current density of 22.59 mA cm −2 at −0.87 V versus reversible hydrogen electrode. The electronic donation of Ag and up‐shifted d‐band center relative to Fermi level within MXene‐regulated Ag−ZnO interfaces contributes the high selectivity of CO. The CO 2 conversion is highly correlated with the dominated linear‐bonded CO intermediate confirmed by in situ infrared spectroscopy. This work enlightens the rational design of unique metal‐oxide interfaces with the regulation of MXene for high‐performance electrocatalysis beyond CO 2 reduction.