Navigating thermal stability intricacies of high-nickel cathodes for high-energy lithium batteries

Zehao Cui, Chen Liu, Feng Wang and Arumugam Manthiram ()
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Zehao Cui: The University of Texas at Austin
Chen Liu: The University of Texas at Austin
Feng Wang: Argonne National Laboratory
Arumugam Manthiram: The University of Texas at Austin

Nature Energy, 2025, vol. 10, issue 4, 490-501

Abstract: Abstract High-nickel oxide cathodes, LiNixM1−xO2 (x ≥ 0.8), are preferred in automotive lithium batteries, but they face thermal instability challenges. Inconsistent literature reports and unstandardized testing protocols further complicate quantitative assessments of the thermal stability of these cathodes. We present here a statistical thermal analysis based on the differential scanning calorimetry measurements of 15 representative cathode materials with different compositions, morphologies and states of charge. The findings reveal that each cathode has a critical state of charge that defines its safe operating limit, which is affected by the metal–oxygen bond strength and surface reactivity. The thermal runaway temperature is dictated by the layered Li1−xNiO2 to LiNi2O4 spinel-like phase transition, which is thermodynamically determined by the metal–oxygen bond covalency and kinetically influenced by the cation mixing and particle size. Raman spectroscopy is used to predict the thermal runaway temperature on the basis of the linear relationship between them. Finally, we propose a thermal stability index to quantify cathode thermal stability as a guide for developing safer high-nickel cathodes.

Date: 2025
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DOI: 10.1038/s41560-025-01731-x

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