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-N-4) 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-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 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-N-4-O active moiety composed of a Ni-N-4 site with an additional oxygen atom that induces an axial traction effect.

Automated summary

An axial traction strategy was developed to optimize the electronic structure of the M-N-4 moiety, leading to atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom embedded within the carbon matrix (Ni-N-4-O/C). This Ni-N-4-O/C electrocatalyst exhibited excellent CO2RR performance with a high CO Faradic efficiency close to 100% at -0.9 V, maintaining the CO FE above 90% in a wide potential window. The superior CO2RR activity is attributed to the axial traction effect induced by the Ni-N-4-O active moiety.