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Electrochemical carbon dioxide (CO2) reduction into value‐added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a FeN4O configuration anchored onto graphene substrate (FeN4OC/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of FeN4O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single‐atomic Fe sites. The FeN4OC/Gr shows excellent performance in the electroreduction of CO2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at −0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h−1. Furthermore, as a cathode catalyst in an aqueous zinc (Zn)‐CO2 battery, the FeN4OC/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm−2 and long‐term stability over 74 h. This work opens up a new route to simultaneously modulate the geometric and electronic structure of single‐atomic catalysts toward efficient CO2 conversion. [ABSTRACT FROM AUTHOR]

Fe N4O C Nanoplates Covalently Bonding on Graphene for Efficient CO2 Electroreduction and Zn CO2 Batteries (Adv. Funct. Zn CO 2 battery, atomically dispersed Fe N 4O, axial coordinations, covalent interactions, electrochemical CO 2 reductions Keywords: Zn CO 2 battery; atomically dispersed Fe N 4O; axial coordinations; covalent interactions; electrochemical CO 2 reductions EN Zn CO 2 battery atomically dispersed Fe N 4O axial coordinations covalent interactions electrochemical CO 2 reductions 1 1 1 07/06/23 20230704 NES 230704 B Electrochemical CO SB 2 sb Reduction b In article number 2300801, Huan Wang and co-workers report a graphene-supported Fe-N SB 4 sb O-C nanoplates electrocatalyst that drives a rechargeable Zn-CO SB 2 sb battery with energy supply and highly efficient conversion of CO SB 2 sb into CO, an important one-carbon building block for the synthesis of long-chain compounds. [Extracted from the article]

Sodium (Na) metal is the most promising alternative anode to metallic lithium for high‐energy batteries due to the low cost and high abundance of Na resources, but it suffers from severe dendritic/mossy growth at high current densities. Understanding Na nucleation/growth mechanism in different electrolyte systems is the key to tackling this issue but is complicated by the structural complexities of existing substrates for Na plating/stripping. Herein, well‐defined planar doped graphene substrates are synthesized as model plating platforms to unravel a binding energy dominant Na nucleation‐growth mode. The dopants (e.g., boron) in doped graphene and the regions close to the dopants possess high binding energies with Na atoms, providing abundant preferential nucleation sites and contributing to uniform Na plating/stripping. Accordingly, the boron‐doped graphene regulated Na anode exhibits long‐term stability at high current densities in both liquid and polymer electrolytes. The results enhance the understanding of Na nucleation/growth for stabilizing Na metal batteries. Planar doped graphene substrates are synthesized to unravel a binding energy dominant sodium (Na) nucleation‐growth mode. The boron (B) dopants in doped graphene and the regions close to the dopants possess high binding energies with Na atoms, providing abundant preferential nucleation sites. Accordingly, the boron‐doped graphene regulated Na anode exhibits long‐term stability at high current densities. [ABSTRACT FROM AUTHOR]