Volume 16, Issue 23 1907368
Full Paper

Elucidation of Active Sites on S, N Codoped Carbon Cubes Embedding Co–Fe Carbides toward Reversible Oxygen Conversion in High-Performance Zinc–Air Batteries

Yuebin Lian

Yuebin Lian

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Kefei Shi

Kefei Shi

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Haojing Yang

Haojing Yang

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Hao Sun

Hao Sun

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Pengwei Qi

Pengwei Qi

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Jing Ye

Jing Ye

Analysis and Testing Center, Soochow University, Suzhou, 215123 China

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Wenbin Wu

Wenbin Wu

KeTai Advanced Materials Co., Ltd, Yichun, Jiangxi, 330800 China

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Zhao Deng

Zhao Deng

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

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Yang Peng

Corresponding Author

Yang Peng

Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou, 215006 P. R. China

Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou, 215006 P. R. China

E-mail: [email protected]

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First published: 05 May 2020
Citations: 83

Abstract

The development of high-performance but low-cost catalysts for the electrochemical oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of central importance for realizing the prevailing application of metal–air batteries. Herein a facile route is devised to synthesize S, N codoped carbon cubes embedding Co–Fe carbides by pyrolyzing the Co–Fe Prussian blue analogues (PBA) coated with methionine. Via the strong metal–sulfur interaction, the methionine coating provides a robust sheath to restrain the cubic morphology of PBA upon pyrolysis, which is proved highly beneficial for promoting the specific surface area and active sites exposure, leading to remarkable bifunctionality of ORR and OER comparable to the benchmarks of Pt/C and RuO2. Further elaborative investigations on the activity origin and postelectrolytic composition unravel that for ORR the high activity is mainly contributed by the S, N codoped carbon shell with the inactive carbide phase converting into carbonate hydroxides. For OER, the embedded Co–Fe carbides transform in situ into layered (hydr)oxides, serving as the actual active sites for promoting water oxidation. Zn–air batteries employing the developed hollow structure as the air cathode catalyst demonstrate superb rechargeability, energy efficiency, as well as portability.

Conflict of Interest

The authors declare no conflict of interest.

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