Volume 17, Issue 52 2104282
Research Article

Structure and Charge Regulation Strategy Enabling Superior Cyclability for Ni-Rich Layered Cathode Materials

Wei Huang

Wei Huang

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

China Automotive Battery Research Institute Co. Ltd, Beijing, 101407 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

General Research Institute for Nonferrous Metals, Beijing, 100088 China

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Wenjin Li

Wenjin Li

College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060 China

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Lve Wang

Lve Wang

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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He Zhu

He Zhu

Department of Physics, City University of Hong Kong, Hong Kong, 999077 China

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Min Gao

Min Gao

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Huan Zhao

Huan Zhao

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

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Jinling Zhao

Jinling Zhao

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Xueling Shen

Xueling Shen

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Xiaodan Wang

Xiaodan Wang

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Ze Wang

Ze Wang

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Chuanlei Qi

Chuanlei Qi

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

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Wei Xiao

Wei Xiao

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

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Lei Yao

Lei Yao

College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060 China

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Jiantao Wang

Corresponding Author

Jiantao Wang

National Power Battery Innovation Center, Grinm Group Corporation Limited, Beijing, 100088 China

School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing, 100083 China

General Research Institute for Nonferrous Metals, Beijing, 100088 China

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

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Weidong Zhuang

Corresponding Author

Weidong Zhuang

China Automotive Battery Research Institute Co. Ltd, Beijing, 101407 China

General Research Institute for Nonferrous Metals, Beijing, 100088 China

Beijing Key Laboratory of Green Recovery and Extraction of Rare and Precious Metals, University of Science and Technology Beijing, Beijing, 100083 China

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

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Xueliang Sun

Corresponding Author

Xueliang Sun

Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9 Canada

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

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First published: 08 October 2021
Citations: 30

Abstract

Ni-rich layered oxides are significantly promising cathode materials for commercial high-energy-density lithium-ion batteries. However, their major bottlenecks limiting their widespread applications are capacity fading and safety concerns caused by their inherently unstable crystal structure and highly reactive surface. Herein, surface structure and bulk charge regulation are concurrently achieved by introducing high-valence Ta5+ ions in Ni-rich cathodes, which exhibit superior electrochemical properties and thermal stability, especially a remarkable cyclic stability with a capacity retention of 80% for up to 768 cycles at a 1C rate versus Li/Li+. Due to the partial Ta enrichment on surface, the regulated surface enables high reversibility of Li+ insertion/extraction by preventing surface Ni reduction in deep charging. Moreover, bulk charge regulation that boosts charge density and its localization on oxygen remarkably suppresses microcracks and oxygen loss, which in turn prevents the fragmentation of the regulated surface and structural degradation associated with oxygen skeleton. This study highlights the significance of an integrated optimization strategy for Ni-rich cathodes and, as a case study, provides a novel and deep insights into the underlying mechanisms of high-valence ions substitution of Ni-rich layered cathodes.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

Research data are not shared.

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