Volume 21, Issue 24 2501965
Research Article

Engineering the Undercoordinated Edge-Rich Single-Crystal Microreactors for High-Performance Lithium─Sulfur Batteries

Mengdi Sun

Mengdi Sun

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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Xincheng Lei

Xincheng Lei

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

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Jiayi Wang

Corresponding Author

Jiayi Wang

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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

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Zhangyong Yan

Zhangyong Yan

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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Chenglin Wei

Chenglin Wei

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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Zefeng Yuan

Zefeng Yuan

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

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Xueyang Gu

Xueyang Gu

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

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Lin Wu

Lin Wu

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

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Ya Hu

Corresponding Author

Ya Hu

Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081 China

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

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Lin Yang

Lin Yang

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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Xin Wang

Corresponding Author

Xin Wang

Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo, 315100 China

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

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Dong Su

Dong Su

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

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Zhongwei Chen

Corresponding Author

Zhongwei Chen

Power Battery and System Research Center, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China

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

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First published: 02 May 2025

Abstract

Lithium─sulfur (Li─S) batteries have garnered extensive research interest due to their high theoretical capacity and cost-effectiveness. However, their practical application is hindered by severe shuttle effects and sluggish conversion kinetics. Here, the development of a novel microreactor composed of undercoordinated edge-rich single-crystal nickel─cobalt bimetallic oxides embedded within a conductive carbon nanotube network (NCO/CNT), as an electrocatalyst for Li─S batteries is reported. The single-crystal bimetallic oxide matrix ensures high structural stability during reactions, while its abundant edge sites provide abundant active catalytic centers. Structural analyses reveal pronounced oxygen undercoordination within NCO/CNT, with these unsaturated sites demonstrating strong adsorption and catalytic activity, effectively promoting sulfur species immobilization and conversion. Complementary theoretical calculations indicate that the unique edge-rich undercoordinated design optimizes the electronic configuration of metal atoms, enhancing electron exchange with sulfur species. Benefiting from these features, Li─S batteries incorporating NCO/CNT achieve an initial discharge capacity of 1327.1 mAh g−1 at 0.2C, and a high areal capacity of 5.4 mAh cm−2 under a sulfur loading of 5.83 mg cm−2, with 96.3% capacity retention after 50 cycles. This work offers insights into the design of high-performance sulfur microreactors, paving the way for efficient and sustainable sulfur electrochemistry.

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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