Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction

Abstract Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M‐N 4 ) to accelerate overall reaction dynamics of the electrochemical CO 2 reduction reaction (CO 2 RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M‐N 4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni‐N 4 ‐O/C). The Ni‐N 4 ‐O/C electrocatalyst exhibited excellent CO 2 RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO 2 RR activity is due to the Ni‐N 4 ‐O active moiety composed of a Ni‐N 4 site with an additional oxygen atom that induces an axial traction effect.