Issue 12, 2024

Rational rock-salt phase engineering of a nickel-rich layered cathode interface for enhanced rate and cycling stability

Abstract

Ni-rich layered cathodes are promising for achieving high energy density, yet suffer from dramatic rate and capacity decay on cycling, which originates from chemo-mechanical failures with fast growth of an electrical and ionic insulating rock-salt phase on the surface. Apart from general approaches of applying inert coating layers, here we regulate the chemistry and structure of the inevitable rock-salt phase, and construct a robust and coherent interface with high electrical and ionic conductivity. Non-metallic N with Al has been co-doped into the interlayer rock-salt phase and the near-surface layered structure. Using atomic-level imaging, spectroscopic analysis, and density-functional-theory calculations, we reveal that Al–N co-doped in the rock-salt phase not only preserves fast Li-transfer pathways, but also increases electron density at the Fermi energy level, enhancing Li-ion diffusion and electron transfer across the rock-salt phase. More importantly, Al–N co-doping stabilizes lattice oxygen (O2−) and reduces interfacial lattice strain, restricting the accelerated accumulation of the rock-salt phase, thereby inhibiting intergranular cracking along cycles. This delicate interface engineering endows LiNi0.83Co0.12Mn0.05O2 with a superior rate capacity of 172.3 mA h g−1 at 3C and a high capacity retention of 96.5% after 200 cycles at 1C. Our findings demonstrate a general strategy with practical significance for mitigating the degradation of Ni-rich layered cathodes.

Graphical abstract: Rational rock-salt phase engineering of a nickel-rich layered cathode interface for enhanced rate and cycling stability

Supplementary files

Article information

Article type
Paper
Submitted
29 Nov 2023
Accepted
08 May 2024
First published
15 May 2024

Energy Environ. Sci., 2024,17, 4283-4294

Rational rock-salt phase engineering of a nickel-rich layered cathode interface for enhanced rate and cycling stability

W. Wang, Y. Shi, P. Li, R. Wang, F. Ye, X. Zhang, W. Li, Z. Wang, C. Xu, D. Xu, Q. Xu and X. Cui, Energy Environ. Sci., 2024, 17, 4283 DOI: 10.1039/D3EE04110G

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