Volume 64, Issue 30 e202503535
Research Article

Utilizing the Mn(II) Dissolution-Induced Vacancy for Optimum Mg2+ Storage of Spinel Mn3O4

Zhongyu Pan

Zhongyu Pan

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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Zhou Jiang

Zhou Jiang

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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Dr. Tingting Qin

Dr. Tingting Qin

Department of Mechanical Engineering, The University of Hong Kong, Hong Kong, 999077 China

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Prof. Dong Wang

Prof. Dong Wang

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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Fuxi Liu

Fuxi Liu

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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He Yang

He Yang

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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Dr. Qing Liang

Dr. Qing Liang

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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Prof. Wei Zhang

Corresponding Author

Prof. Wei Zhang

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

E-mail: [email protected]

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Prof. Weitao Zheng

Prof. Weitao Zheng

Key Laboratory of Automobile Materials MOE, School of Materials Science & Engineering, Electron Microscopy Center, International Center of Future Science, Changbaishan Laboratory, Jilin University, Changchun, 130012 China

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First published: 16 May 2025
Citations: 1

Graphical Abstract

There are two significant factors necessary for the cathode materials of aqueous Mg-ion energy storage devices as follows: one is the storage mechanism of Mg2+ that can achieve enhanced Mg2+ diffusion kinetics and bring higher power density; the other is the high structural stability to achieve long lifespan. The tetrahedral vacancy reversible insertion/extraction mechanism by Mn(II) dissolution and optimize the integrity of the spinel framework is a powerful strategy to achieve Mg2+ energy storage system with high rate performance and long lifespan.

Abstract

Manganese-based oxide can theoretically exert the multivalent advantages of an aqueous magnesium-ion cathode due to its redox activity and abundant crystal structure. However, sluggish diffusion kinetics of Mg2+ and Mn dissolution limit the rate performance and structure stability. Herein, we successfully utilize the notorious dissolution of Mn(II) tetrahedral site contributed vacancies for packaging optimum Mg2+ storage of a popular spinel Mn3O4 electrode. Such mechanism reverses the sluggish diffusion kinetics. Moreover, merited by the common ion effect and drug dissolution, a suitable preaddition of Mn2+ to electrolyte inhibit Mn(III) dissolution and optimize the integrity of the spinel framework. Impressively, the cathode achieves a reversible capacity of 310 mAh g−1 and a stable cycle performance of 2000 cycles with 94.9% retention. Our research shows that reversible insertion/extraction at vacancies and effective stabilization of spinel framework is a powerful strategy to achieve Mg2+ ion energy storage system with high rate performance and long lifespan.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in Supporting Information of this article.

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