Topotaxially grown composite cathodes for cobalt-free high-energy long-life Li-ion batteries

Junyi Yao, Sizhan Liu, Wujun Zhang, Lijun Wu, Zhenjie Zhang, Ping He, Yanbin Shen, Liwei Chen (), Mingyuan Ge, Lu Ma, Xiaotian Zhu, Kaihua Xu, Kun Zhang, Feng Wang, Jianqing Zhao () and Jianming Bai ()
Additional contact information
Junyi Yao: Soochow University, College of Energy, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Sizhan Liu: Brookhaven National Laboratory, Interdisciplinary Science Department
Wujun Zhang: Chinese Academy of Sciences, i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO)
Lijun Wu: Brookhaven National Laboratory, Condensed Matter Physics and Materials Science Division
Zhenjie Zhang: Nanjing University, Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructures
Ping He: Nanjing University, Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructures
Yanbin Shen: Chinese Academy of Sciences, i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO)
Liwei Chen: Chinese Academy of Sciences, i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO)
Mingyuan Ge: Brookhaven National Laboratory, National Synchrotron Light Source II
Lu Ma: Brookhaven National Laboratory, National Synchrotron Light Source II
Xiaotian Zhu: Soochow University, College of Energy, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Kaihua Xu: GEM Co., Ltd.
Kun Zhang: GEM Co., Ltd.
Feng Wang: Argonne National Laboratory, Applied Materials Division
Jianqing Zhao: Soochow University, College of Energy, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies
Jianming Bai: Brookhaven National Laboratory, National Synchrotron Light Source II

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract The vehicle industry’s increasing demand for electrification necessitates the removal of expensive and rare cobalt from current high-energy batteries. However, eliminating cobalt poses challenges due to its vital role in maintaining the layered structural ordering and cycling stability of commonly used Li(NiMnCo)O2 cathodes. As an alternative to conventional layered oxide designs, we report a lithium nickelate cathode with a composite structure comprising major stoichiometric layered and minor rocksalt phases within the same oxygen lattice. This material outperforms conventional designs by maintaining stable battery operation at voltages up to 4.8 V vs. Li|Li+, with 88% capacity retention after 1000 cycles at 2C. The topotaxial-growth-enabled interlock between the two components mitigates chemo-mechanical degradation, offering a promising pathway to cobalt-free cathodes. Additionally, we reveal a miscibility gap in the Li-Ni-O system that enables kinetic adjustment of composition and structure during sintering, thereby tuning the functionality of high-energy cathodes.

Date: 2025
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DOI: 10.1038/s41467-025-63258-9

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