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

Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M‐N4) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M‐N4 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‐N4‐O/C). The Ni‐N4‐O/C electrocatalyst exhibited excellent CO2RR 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 CO2RR activity is due to the Ni‐N4‐O active moiety composed of a Ni‐N4 site with an additional oxygen atom that induces an axial traction effect. An axial traction strategy is presented to reduce the energy barrier of the dynamic activation process over the M‐N4 structure for boosting CO2RR activity.