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.