High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material

By Yuwei Mao, Xuelong Wang, Sihao Xia, Kai Zhang, Chenxi Wei, Seong‐Min Bak, Zulipiya Shadike, Xuejun Liu, Yang Yang, Rong Xu and 9 more. Advanced Functional Materials, 2019

292 citations recorded by the source corpus.

Nickel‐rich layered materials LiNi1‐x‐yMnxCoyO2 are promising candidates for high‐energy‐density lithium‐ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially with high‐voltage charging. It is critical to have a mechanistic understanding of such fade. Herein, synchrotron‐based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi0.6Mn0.2Co0.2O2 material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high‐voltage charging. Nano‐resolution 3D transmission X‐ray microscopy data analyzed by machine learning methodology reveal that high‐voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro‐cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress‐induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crack problem in these materials.

Subfields: Electrical and Electronic Engineering, Mechanical Engineering

View Paper: https://www.semanticscholar.org/paper/02174db15657f9bf474bb52a4d0aecfb0f7b7e22

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In Electrical and Electronic Engineering

1. K. Zhao
2. Feng Lin

In Mechanical Engineering

1. Fei Yin
2. Peter Cloetens
3. Rong Xu
4. Yijin Liu
5. Pengfei Liu
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7. Yang Yang
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Citations in the corpus

• Heterogeneous Damage in Li-Ion Batteries: Experimental Analysis and Theoretical Modeling (2019, background): “The experimental results in this paper were not included in our previous work ( Yang et al., 2019 ).”