Linking Transport with Intercalation Mechanisms, Cracking, and Dendrite Formation in Conventional and Solid-State Batteries.
Clare Grey a
a University of Cambridge, JJ Thomson Avenue, Cambridge, United Kingdom
Proceedings of 24th International Conference on Solid State Ionics (SSI24)
London, United Kingdom, 2024 July 14th - 19th
Organizers: John Kilner and Stephen Skinner
Keynote, Clare Grey, presentation 480
Publication date: 10th April 2024

This talk will describe how a combination of NMR to measure transport, X-ray diffraction to measure phase segregation within the bulk, optical measurements and electron microscopy to explore processes at the particle level, and continuum modeling to tie transport with particle level observations, can be used to study electrode material function and failure. First, NMR measurements provide hopping frequencies and diffusion coefficients. Second, operando diffraction measurements provide evidence for solid solution vs two phase behaviour as a function of cycling. New optical measurements allow phase transformation and phase fronts to be visualized directly. The processes that underpin the various phase fronts can then be explored via simulations.  This is illustrated with nickel rich layered cathode materials such as NMC-811.  The approach is extended to study the end member of this series LiNiO2 where the effect of phase transitions at the top of charge (i.e., when most of the Li is removed), has significant implications for particle degradation via processes such as cracking (along with oxygen loss).  Finally, the role that transport, grain boundaries and surface impurities have on dendrite formation in oxide-based solid-state battery electrolytes will be discussed. 

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