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Research Article

A pH-universal ORR catalyst with atomic Fe-heteroatom (N, S) sites for high-performance Zn-air batteries

Le Li1,2, Na Li1, Jia-Wei Xia1, Shi-Long Zhou1, Xing-Yue Qian1, Feng-Xiang Yin1, Guo-Hong Dai1, Guang-Yu He1( ), Hai-Qun Chen1( )
Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China
Jiangsu Urban and Rural Construction Vocational College, Changzhou 213147, China
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Graphical Abstract

Benefiting from unique FeN3S moieties with optimized intrinsic activity, a high specific surface area for adequate active sites exposure, and a hierarchical porous structure for rapid ions/mass transfer, the resultant Fe-SAs/S,N-C/rGO catalyst exhibits satisfactory oxygen reduction reaction (ORR) activity at a wide pH range. Notably, the corresponding liquid and flexible solid-state Zn-air batteries manifest excellent battery performance.

Abstract

Developing innovative, easy-to-manufacture, and non-Pt-group-metal (non-PGM) electrocatalysts is essential for the highly efficient oxygen reduction reaction (ORR). Herein, we report a self-sacrificing post-synthetic strategy to synthesize highly loaded Fe-isolated single atoms anchored on the hierarchical porous N,S co-doped carbon matrix (Fe-SAs/S,N-C/rGO). The optimized Fe-SAs/S,N-C/rGO exhibits excellent ORR activity in the pH-universal range with half-wave potentials of 0.89, 0.80, and 0.60 V in alkaline, acidic, and neutral media, comparable to the commercial Pt/C (0.85, 0.81, and 0.64 V, respectively). The homemade liquid Zn-air battery (ZAB) with Fe-SAs/S,N-C/rGO as the cathode catalyst displays an open-circuit voltage (OCV) of ~ 1.61 V, discharging specific capacity of 817.23 mAh·g−1, and long-term durability of ~ 1865 cycles, outperforming those of the device with commercial Pt/C+RuO2 (1.49 V, 657.32 mAh·g−1, and ~ 120 cycles, respectively). Intriguingly, the corresponding flexible solid-state ZAB delivers satisfactory OCV, peak power density, foldability, and cycling stability at room temperature, as well as adaptability at a low temperature of −10 °C. Besides, density functional theory (DFT) calculation reveals that the atomic FeN3S moieties in Fe-SAs/S,N-C/rGO can cause charge redistribution and lower the binding strength of oxygen-containing intermediates, resulting in accelerated ORR kinetics and optimized catalytic activity. This work provides insights into experimental and theoretical guidance towards non-PGM electrocatalysts for efficient energy conversion.

Keywords

heteroatom dopantsingle-atom electrocatalystFeN3S sitesZn-air batterydensity functional theory (DFT) study

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Nano Research
Volume 16 Issue 7,
July 2023
Pages 9416-9425
DOI: 10.1007/s12274-023-5625-y
Cite this article:
Li L, Li N, Xia J-W, et al. A pH-universal ORR catalyst with atomic Fe-heteroatom (N, S) sites for high-performance Zn-air batteries. Nano Research, 2023, 16(7): 9416-9425. https://doi.org/10.1007/s12274-023-5625-y
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Received: 23 January 2023
Revised: 23 February 2023
Accepted: 27 February 2023
Published: 30 March 2023
© Tsinghua University Press 2023
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