Altering the Symmetry of Fe–N–C by Axial Cl‐Mediation for High‐Performance Zinc–Air Batteries

Fe-N-C catalyst is acknowledged as a promising alternative for the state-of-the-art Pt/C in oxygen reduction reaction (ORR) toward cutting-edge electrochemical energy conversion/storage applications. Herein, a "Cl-mediation" strategy is proposed on Fe-N-C for modulating the catalyst's electronic structure toward achieving remarkable ORR activity. By coordinating axial Cl atoms to iron phthalocyanine (FePc) molecules on carbon nanotubes (CNTs) matrix, a Cl-modulated Fe-N-C (FePc-Cl-CNTs) catalyst is synthesized. The as-prepared FePc-Cl-CNTs exhibit an improved ORR activity with a half-wave potential of 0.91 V versus RHE in alkaline solution, significantly outperforming the parent FePc-CNTs (0.88 V versus RHE). The advanced nature of the as-prepared FePc-Cl-CNTs is evidenced by a configured high-performance rechargeable Zn-air battery, which operates stably for over 150 h. The experiments and density functional theory calculations unveil that axial Cl atoms induce the transformation of FePc from its original D<sub>4h</sub> to C<sub>4v</sub> symmetry, effectively altering the electrons distribution around the Fe-center, by which it optimizes *OH desorption and subsequently boosts the reaction kinetics. This work paves ways for resolving the dilemma of Fe-N-C catalysts' exploration via engineering Fe-N-C configuration.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-04-15
DOI
https://doi.org/10.1002/anie.202504923
Citations
29
Primary Topic
Electrocatalysts for Energy Conversion
Type
article
Field-Weighted Citation Impact
10.54

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article

Altering the Symmetry of Fe–N–C by Axial Cl‐Mediation for High‐Performance Zinc–Air Batteries

Yuxiao Liu, Haowei Yang, Chundong Wang, Dingsheng S. Wang et al.
29 citations
Angewandte Chemie International Edition
Electrocatalysts for Energy Conversion
10.54
article

Altering the Symmetry of Fe–N–C by Axial Cl‐Mediation for High‐Performance Zinc–Air Batteries

Yuxiao Liu, Haowei Yang, Chundong Wang, Dingsheng S. Wang, Libo Sun, M. Bououdina, Jianrong Zeng, Mengni Liu, Xin Wang, Linfeng Li, Xuefeng Zhang, Deli Wang, Xinying Xue, Rony Snyders
article en
29 citations

Abstract

Fe-N-C catalyst is acknowledged as a promising alternative for the state-of-the-art Pt/C in oxygen reduction reaction (ORR) toward cutting-edge electrochemical energy conversion/storage applications. Herein, a "Cl-mediation" strategy is proposed on Fe-N-C for modulating the catalyst's electronic structure toward achieving remarkable ORR activity. By coordinating axial Cl atoms to iron phthalocyanine (FePc) molecules on carbon nanotubes (CNTs) matrix, a Cl-modulated Fe-N-C (FePc-Cl-CNTs) catalyst is synthesized. The as-prepared FePc-Cl-CNTs exhibit an improved ORR activity with a half-wave potential of 0.91 V versus RHE in alkaline solution, significantly outperforming the parent FePc-CNTs (0.88 V versus RHE). The advanced nature of the as-prepared FePc-Cl-CNTs is evidenced by a configured high-performance rechargeable Zn-air battery, which operates stably for over 150 h. The experiments and density functional theory calculations unveil that axial Cl atoms induce the transformation of FePc from its original D<sub>4h</sub> to C<sub>4v</sub> symmetry, effectively altering the electrons distribution around the Fe-center, by which it optimizes *OH desorption and subsequently boosts the reaction kinetics. This work paves ways for resolving the dilemma of Fe-N-C catalysts' exploration via engineering Fe-N-C configuration.

Angewandte Chemie International EditionVol. 64(26)
Shihezi University (CN), University of Mons (BE), Central South University (CN), Prince Sultan University (SA), City University of Hong Kong (HK), Chinese Academy of Sciences (CN), Shanghai Advanced Research Institute (CN), Shanghai Institute of Applied Physics (CN), Materia Nova (BE), Huazhong University of Science and Technology (CN), Tsinghua University (CN)
City University of Hong Kong, Salt Science Research Foundation, National Natural Science Foundation of China, Fonds De La Recherche Scientifique - FNRS, Fonds Wetenschappelijk Onderzoek, Huazhong University of Science and Technology, Prince Sultan University
Affordable and clean energy
Openalex Percentile: Top 1%
Electrocatalysts for Energy Conversion
10.54
DOIOpen Access PDFOpenAlex
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