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

Yao, Junyi; Liu, Sizhan; Zhang, Wujun; Wu, Lijun; Zhang, Zhenjie; He, Ping; Shen, Yanbin; Chen, Liwei; Ge, Mingyuan; Ma, Lu; Zhu, Xiaotian; Xu, Kaihua; Zhang, Kun; Wang, Feng; Zhao, Jianqing; Bai, Jianming

doi:10.1038/s41467-025-63258-9

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

Journal Article · Thu Nov 20 00:00:00 EST 2025 · Nature Communications

DOI:https://doi.org/10.1038/s41467-025-63258-9· OSTI ID:3010959

Yao, Junyi ^[1]; ^[2]; Zhang, Wujun ^[3]; ^[2]; Zhang, Zhenjie ^[4]; ^[4]; ^[3]; ^[5]; ^[6]; ^[6]; Zhu, Xiaotian ^[7]; Xu, Kaihua ^[8]; Zhang, Kun ^[8]; ^[9]; ^[10]; ^[6]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States); Soochow University, Suzhou (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Chinese Academy of Sciences (CAS), Suzhou (China)
Nanjing University (China)
Shanghai Jiao Tong University (China); Chinese Academy of Sciences (CAS), Suzhou (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Soochow University, Suzhou (China)
GEM Co., Ltd., Shenzhen (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Soochow University, Suzhou (China); Jiangsu Zoolnasm Technology Co., LTD, Suzhou (China)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 3010959

Report Number(s):: BNL--229276-2025-JAAM

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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