Volume 136, Issue 1 e202316314
Forschungsartikel

Engineering Electronic Structure of Nitrogen-Carbon Sites by sp3-Hybridized Carbon and Incorporating Chlorine to Boost Oxygen Reduction Activity

Xueting Feng

Xueting Feng

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

These authors contributed equally to this work.

Contribution: Writing - original draft (lead)

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Guanzhen Chen

Guanzhen Chen

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

These authors contributed equally to this work.

Contribution: Writing - original draft (equal)

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Zhibo Cui

Zhibo Cui

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - original draft (supporting)

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Rong Qin

Rong Qin

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - original draft (supporting)

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Wensheng Jiao

Wensheng Jiao

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - original draft (supporting)

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Zeyi Huang

Zeyi Huang

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - original draft (supporting)

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Ziang Shang

Ziang Shang

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - original draft (supporting)

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Dr. Chao Ma

Dr. Chao Ma

Department of Chemistry, Tsinghua University, Beijing, 100084 China

Contribution: Writing - original draft (supporting)

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Dr. Xusheng Zheng

Dr. Xusheng Zheng

National Synchrotron Radiation Laboratory University of Science and Technology of China, Hefei, Anhui, 230029 China

Contribution: Writing - original draft (supporting)

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Prof. Yunhu Han

Corresponding Author

Prof. Yunhu Han

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

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Prof. Wei Huang

Corresponding Author

Prof. Wei Huang

Institute of Flexible Electronics (IFE), Ningbo Institute, and Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072 China

Contribution: Writing - review & editing (supporting)

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First published: 30 November 2023
Citations: 4

Abstract

Development of efficient and easy-to-prepare low-cost oxygen reaction electrocatalysts is essential for widespread application of rechargeable Zn-air batteries (ZABs). Herein, we mixed NaCl and ZIF-8 by simple physical milling and pyrolysis to obtain a metal-free porous electrocatalyst doped with Cl (mf-pClNC). The mf-pClNC electrocatalyst exhibits a good oxygen reduction reaction (ORR) activity (E1/2=0.91 V vs. RHE) and high stability in alkaline electrolyte, exceeding most of the reported transition metal carbon-based electrocatalysts and being comparable to commercial Pt/C electrocatalysts. Likewise, the mf-pClNC electrocatalyst also shows state-of-the-art ORR activity and stability in acidic electrolyte. From experimental and theoretical calculations, the better ORR activity is most likely originated from the fact that the introduced Cl promotes the increase of sp3-hybridized carbon, while the sp3-hybridized carbon and Cl together modify the electronic structure of the N-adjacent carbons, as the active sites, while NaCl molten-salt etching provides abundant paths for the transport of electrons/protons. Furthermore, the liquid rechargeable ZAB using the mf-pClNC electrocatalyst as the cathode shows a fulfilling performance with a peak power density of 276.88 mW cm−2. Flexible quasi-solid-state rechargeable ZAB constructed with the mf-pClNC electrocatalyst as the cathode exhibits an exciting performance both at low, high and room temperatures.

Conflict of interest

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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