Volume 64, Issue 30 e202502725
Research Article

Mechanically and Chemically Co-Robust Ni-Rich Cathodes with Ultrahigh Capacity and Prolonged Cycle Life

Bo Wang

Bo Wang

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

These authors contributed equally to this work.

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Kuo Li

Kuo Li

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

These authors contributed equally to this work.

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Ge Xu

Ge Xu

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

These authors contributed equally to this work.

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Zihan Zhang

Zihan Zhang

Department of Mechanics, School of Aerospace Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074 P.R. China

These authors contributed equally to this work.

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Xinxin Wang

Xinxin Wang

Department of Mechanics, School of Aerospace Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074 P.R. China

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Jun Sun

Jun Sun

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

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Yijun Song

Yijun Song

School of Materials Science and Engineering, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580 P.R. China

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Xuedong Zhang

Xuedong Zhang

Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University, Xiangtan, 411105 P.R. China

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Yali Liang

Yali Liang

Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 P.R. China

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Dejie Kong

Dejie Kong

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

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Yuan Qiu

Yuan Qiu

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

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Qipeng Teng

Qipeng Teng

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

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Xin Cui

Xin Cui

Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University, Xiangtan, 411105 P.R. China

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Jingzhao Chen

Jingzhao Chen

Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 P.R. China

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Jun Zhao

Jun Zhao

Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 P.R. China

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Jing Wang

Jing Wang

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

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Hui Yang

Corresponding Author

Hui Yang

Department of Mechanics, School of Aerospace Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074 P.R. China

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

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Jianyu Huang

Corresponding Author

Jianyu Huang

Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 P.R. China

Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University, Xiangtan, 411105 P.R. China

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

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Yongfu Tang

Corresponding Author

Yongfu Tang

Hebei Key Laboratory of Applied Chemistry, State Key Laboratory of Metastable Materials Science and Technology (MMST), Yanshan University, Qinhuangdao, 066004 P.R. China

Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 P.R. China

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

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First published: 16 April 2025
Citations: 1

Graphical Abstract

A comprehensive understanding of the concurrent capacity and stability enhancement mechanisms attributed to Nb-doping and highlights the significant potential of the synergistic regulation of mechanical and chemical coupling in improving the capacity and lifespan of NRLOs by Nb-doping.

Abstract

Ni-rich layered oxide (NRLO) materials are considered highly promising cathode for lithium-ion batteries. However, their practical application is limited by capacity loss and interface instability caused by chemical and mechanical failure during cycling. Doping has been identified as a direct and effective method to address these challenges. However, mechanistic understanding of doping enhanced electrochemical performance is still unclear. In this study, the introduction of high-valent Nb ions was employed to achieve mechanical–chemical coupling regulation, thereby concurrently improving the capacity and cycle life of NRLO. First, Nb5+ doping was conducted to refine secondary grains, achieving a “grain refinement” effect similar to that in ceramics and alloys, while further stabilizing the grain boundaries. The intergrain fusion structure of NCM811-0.5Nb effectively dissipates lattice strain under highly delithiated state, suppresses oxygen loss, and prevents cracks that lead to fracture during cycling. Moreover, Nb doping stabilizes the monoclinic phase during phase transitions and promotes the formation of highly stable spinel twin boundaries after cycling. This effectively reduces the Li diffusion barrier, leading to improved reversible specific capacity and rate capability. Lastly, the strong Nb─O bonding restrains oxygen release and transition metal/Li antisite mixing, thus mitigate rock-salt phase formation. This study demonstrates a comprehensive understanding of the concurrent capacity and stability enhancement mechanisms attributed to Nb-doping and highlights the significant potential of the synergistic regulation of mechanical and chemical coupling in improving the capacity and lifespan of NRLOs by Nb-doping.

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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