Oxygen‐Bridged Indium‐Nickel Atomic Pair as Dual‐Metal Active Sites Enabling Synergistic Electrocatalytic CO2 Reduction

Abstract Single‐atom catalysts offer a promising pathway for electrochemical CO2 conversion. However, it is still a challenge to optimize the electrochemical performance of dual‐atom catalysts. Here, an atomic indium‐nickel dual‐sites catalyst bridged by an axial oxygen atom (O‐In‐N6‐Ni moiety) was anchored on nitrogenated carbon (InNi DS/NC). InNi DS/NC exhibits superior CO selectivity with Faradaic efficiency higher than 90 % over a wide potential range from −0.5 to −0.8 V versus reversible hydrogen electrode (vs. RHE). Moreover, an industrial CO partial current density up to 317.2 mA cm−2 is achieved at −1.0 V vs. RHE in a flow cell. In situ ATR‐SEIRAS combined with theory calculations reveal that the synergistic effect of In‐Ni dual‐sites and O atom bridge not only reduces the reaction barrier for the formation of *COOH, but also retards the undesired hydrogen evolution reaction. This work provides a feasible strategy to construct dual‐site catalysts towards energy conversion.