Issue 13, 2022

Promoting oxygen reduction via crafting bridge-bonded oxygen ligands on a single-atom iron catalyst

Abstract

Single-atom Fe–N–C materials with Fe–N4 coordination structures, hailed as promising catalysts, are prohibited by the severe aggregation and migration of metal atoms. Although bonding-confinement strategies can be used to effectively regulate and strengthen the coordination of isolated metal atoms, the precise control of the coordination environment of metal centers remains a challenge. Herein, we report a rational strategy by which to bond iron phthalocyanine (FePc) on pre-synthesized Fe–N–C materials to further obtain anatomically dispersed Fe–N4 catalysts. The axial coordination of O-FeN4 sites to form a Fe–O–Fe bridge bond lowers the overpotential for the oxygen reduction reaction (ORR). Incorporation of the O atom stimulates the adsorbed O2 to obtain more electrons, thereby enhancing the adsorption and activation of O2. The catalyst demonstrates a half-wave potential of 0.866 V (versus RHE) and kinetic current density of 11.49 mA cm−2, significantly outperforming commercial Pt/C. The primary Zn–air battery assembled with such a catalyst exhibits a high current density of 136 mA cm−2 @ 1.0 V and a maximum power density of 205 mW cm−2, supporting its potential feasibility in practical applications. Our findings provide a new avenue for tuning the coordination environment of single-atom catalysts to enhance their ORR activity.

Graphical abstract: Promoting oxygen reduction via crafting bridge-bonded oxygen ligands on a single-atom iron catalyst

Supplementary files

Article information

Article type
Research Article
Submitted
28 Mar 2022
Accepted
21 May 2022
First published
23 May 2022

Inorg. Chem. Front., 2022,9, 3306-3318

Promoting oxygen reduction via crafting bridge-bonded oxygen ligands on a single-atom iron catalyst

C. Xu, Y. Si, B. Hu, X. Xu, B. Hu, Y. Jiang, H. Chen, C. Guo, H. Li and C. Chen, Inorg. Chem. Front., 2022, 9, 3306 DOI: 10.1039/D2QI00668E

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