Propagation topography of redox phase transformations in heterogeneous layered oxide cathode materials

Nature Communications
Linqin MuFeng Lin

Abstract

Redox phase transformations are relevant to a number of metrics pertaining to the electrochemical performance of batteries. These phase transformations deviate from and are more complicated than the conventional theory of phase nucleation and propagation, owing to simultaneous changes of cationic and anionic valence states as well as the polycrystalline nature of battery materials. Herein, we propose an integrative approach of mapping valence states and constructing chemical topographies to investigate the redox phase transformation in polycrystalline layered oxide cathode materials under thermal abuse conditions. We discover that, in addition to the three-dimensional heterogeneous phase transformation, there is a mesoscale evolution of local valence curvatures in valence state topographies. The relative probability of negative and positive local valence curvatures alternates during the layered-to-spinel/rocksalt phase transformation. The implementation of our method can potentially provide a universal approach to study phase transformation behaviors in battery materials and beyond.

References

Aug 7, 2007·Physical Review Letters·Lei ZhangQiang Du
Feb 22, 2012·Analytical and Bioanalytical Chemistry·Yijin LiuPiero Pianetta
May 23, 2013·Nature Communications·Timofey FrolovYuri Mishin
Jun 8, 2013·Chemistry of Materials : a Publication of the American Chemical Society·Ulrike BoesenbergJordi Cabana
Feb 25, 2014·Nature Communications·Feng LinHuolin L Xin
Jan 27, 2015·Scientific Reports·Kuppan SaravananGuoying Chen
Oct 26, 2016·Nature Materials·Hadi TavassolAndrew A Gewirth
Dec 9, 2016·Proceedings of the National Academy of Sciences of the United States of America·H JangJ-S Lee

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Citations

May 10, 2020·Journal of Synchrotron Radiation·Chenxi WeiPiero Pianetta
Jan 1, 2021·Advanced Materials·Jun MeiZongyou Yin
Jul 18, 2019·ACS Applied Materials & Interfaces·Haowei ZhaiYuan Yang

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Methods Mentioned

BETA
electron microscopy
X-ray
transmission electron microscopy

Software Mentioned

Wizard
TXM

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