Volume 137, Issue 26 e202504923
Forschungsartikel

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

Mengni Liu

Mengni Liu

Department of Physics, College of Science, Shihezi University, Xinjiang, 832003 P.R. China

School of Integrated Circuits, State Key Laboratory of New Textile Materials and Advanced Processing, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

Both authors contributed equally to this work.

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Yuxiao Liu

Yuxiao Liu

School of Integrated Circuits, State Key Laboratory of New Textile Materials and Advanced Processing, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

Both authors contributed equally to this work.

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Xia Zhang

Xia Zhang

School of Integrated Circuits, State Key Laboratory of New Textile Materials and Advanced Processing, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

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Linfeng Li

Linfeng Li

School of Integrated Circuits, State Key Laboratory of New Textile Materials and Advanced Processing, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

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Xinying Xue

Corresponding Author

Xinying Xue

Department of Physics, College of Science, Shihezi University, Xinjiang, 832003 P.R. China

E-mail: [email protected]; [email protected]; [email protected]

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Muhammad Humayun

Muhammad Humayun

Energy, Water and Environment Lab, College of Humanities and Sciences, Prince Sultan University, Riyadh, 11586 Saudi Arabia

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Haowei Yang

Haowei Yang

School of Materials Science and Engineering, Central South University, Changsha, 410083 P.R. China

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Libo Sun

Libo Sun

Department of Chemistry, City University of Hong Kong, Hong Kong, 999077 P. R. China

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Mohamed Bououdina

Mohamed Bououdina

Energy, Water and Environment Lab, College of Humanities and Sciences, Prince Sultan University, Riyadh, 11586 Saudi Arabia

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Jianrong Zeng

Jianrong Zeng

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204 P.R. China

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Deli Wang

Deli Wang

School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

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Rony Snyders

Rony Snyders

Chimie des Interactions Plasma Surfaces (ChIPS), University of Mons, Mons, 7000 Belgium

Materia Nova Research Center, Mons, B-7000 Belgium

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Dingsheng Wang

Dingsheng Wang

Department of Chemistry, Tsinghua University, Beijing, 100084 P.R. China

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Xin Wang

Corresponding Author

Xin Wang

Department of Chemistry, City University of Hong Kong, Hong Kong, 999077 P. R. China

E-mail: [email protected]; [email protected]; [email protected]

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Chundong Wang

Corresponding Author

Chundong Wang

School of Integrated Circuits, State Key Laboratory of New Textile Materials and Advanced Processing, Huazhong University of Science and Technology, Wuhan, 430074 P.R. China

Energy, Water and Environment Lab, College of Humanities and Sciences, Prince Sultan University, Riyadh, 11586 Saudi Arabia

E-mail: [email protected]; [email protected]; [email protected]

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First published: 15 April 2025

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 D4h to C4v 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.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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