Exceptional layered cathode stability at 4.8 V via supersaturated high-valence cation design

Hengyi Liao, Yufeng Tang, Wenqin Ma, Yong Liu, Yanhao Dong () and Fuqiang Huang ()
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Hengyi Liao: Peking University
Yufeng Tang: Chinese Academy of Sciences
Wenqin Ma: Chinese Academy of Sciences
Yong Liu: Shanghai Institute of Space Power-Sources
Yanhao Dong: Tsinghua University
Fuqiang Huang: Shanghai Jiao Tong University

Nature Energy, 2025, vol. 10, issue 9, 1107-1115

Abstract: Abstract High-energy-density lithium-ion batteries for extreme conditions require cathodes that remain stable under harsh operation, including ultrahigh cutoff voltage and extreme temperatures. For Ni-rich layered cathodes, raising the charge voltage from 4.3 V to 4.8 V (versus Li+/Li) increases the energy density, yet this sacrifices cycling stability and remains challenging. Here we report a dopant-pairing method that achieves highly enriched Ti4+ (~9-nm surface layer) in LiNi0.8Co0.1Mn0.1O2 facilitated by Na+, enabling significantly enhanced high-voltage cyclability. Such high surface Ti4+ concentrations are unattainable without pairing Na+, representing a form of supersaturation within the layered cathode matrix. The enhanced stability is linked to improved structural integrity and reduced cathode–electrolyte side reactions (for example, O2 and CO2 evolution). In addition, ion transport is better preserved even after prolonged cycling at 4.8 V. This work highlights the power of supersaturated high-valence d0 cation Mz+ (z ≥ 4) in modifying the cathode–electrolyte interactions and degradation pathway.

Date: 2025
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DOI: 10.1038/s41560-025-01831-8

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