Volume 64, Issue 30 e202501539
Research Article

Layered-Spinel Heterogeneous Structure and Oxygen Vacancies Enable Superior Electrochemical Performance for Li-Rich Cathodes

Pengkun Yang

Pengkun Yang

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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Dr. Long Shang

Dr. Long Shang

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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Dr. Huimin Wang

Dr. Huimin Wang

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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Prof. Zhenhua Yan

Prof. Zhenhua Yan

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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Prof. Kai Zhang

Prof. Kai Zhang

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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Prof. Yixin Li

Corresponding Author

Prof. Yixin Li

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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

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Prof. Jun Chen

Corresponding Author

Prof. Jun Chen

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry, Nankai University, Tianjin, 300071 P.R. China

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

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First published: 25 May 2025

Graphical Abstract

A multifunctional interfacial layer of layered-spinel heterogeneous structure and oxygen vacancies was formed on the surface of LRMOs, which improved the structural stability and the reversibility of anion redox reaction. The treated cathode features high initial capacity of 314.5 mAh g−1 with a coulombic efficiency of 88.3%. When cycling at 1 C, the cathode shows a high capacity retention of 87.9% with a small voltage decay of 1.26 mV per cycle.

Abstract

Lithium-rich manganese-based oxides (LRMOs) materials are considered to be the next-generation cathode for high-energy lithium-ion/metal batteries owing to their superior specific capacity, high operation voltage, and low cost. However, the commercial application of LRMOs is constrained by the surface structure degradation and lattice oxygen release, resulting in low initial coulombic efficiency (ICE) and rapid voltage and capacity decay. Herein, we propose a facile sorbic acid-assisted surface treatment strategy to construct homogeneous multifunctional interface layers composed of layered-spinel heterogeneous structure and oxygen vacancies on the surface of LRMOs, which enhance the structure stability and improve the activity and reversibility of the anionic oxygen redox reactions. The multifunctional interfacial layers effectively suppress irreversible oxygen release and alleviate unfavorable layered-spinel phase transformation. As a consequence, the treated LRMOs cathode displays improved ICE of 88.3%, high capacity retention rate (87.9% at 1 C after 150 cycles) and low voltage decay ratio (1.26 mV per cycle). These findings provide a valuable new idea to improve the comprehensive electrochemical performance of LRMOs through multi-strategy synergistic interface engineering techniques.

Conflict of Interests

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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