Coordination environment engineering to boost electrocatalytic CO2 reduction performance by introducing boron into single-Fe-atomic catalyst

Electrocatalytic CO2 reduction reaction (CRR), powered by renewable energy sources, is a promising route to address energy and environmental issues. Herein, we fabricate single atomic Fe sites anchored on B and N co-doped carbon (Fe-SA/BNC), which showed excellent CRR activity, achieving a highest Faradaic efficiency of ~94% at -0.7 V versus reversible hydrogen electrode. The performance is much better than that of the B-free sample. Furthermore, an outstanding current density of ~130 mA cm(-2), as well as ~99% Faradaic efficiency, has been achieved using the membrane electrode assembly (MEA). Details of density functional theory (DFT) calculations revealed that the introduction of B was beneficial for the desorption of *CO. The Zn-CO2 battery was then assembled, which reached a high peak power density of 1.18 mW cm(-2) at a current density of 4 mA cm(-2), as well as showing remarkable stability for CO production.

Automated summary

In this study, Fe-SA/BNC material was successfully fabricated and exhibited excellent CO2 reduction reaction activity, achieving remarkable current density and Faradaic efficiency through MEA. Density functional theory (DFT) calculations revealed the positive effect of introducing B on the desorption of *CO. Furthermore, the assembled Zn-CO2 battery demonstrated outstanding peak power density and stability for CO production.