First published:

Last Edited:

Number of edits:

  • title: Operando monitoring of single-particle kinetic state-of-charge heterogeneities and cracking in high-rate Li-ion anodes
  • authors: Alice J. Merryweather, Quentin Jacquet, Steffen P. Emge, Christoph Schnedermann, Akshay Rao, Clare P. Grey
  • year: 2022
  • 10.1038/s41563-022-01324-z

To rationalize and improve the performance of newly developed high-rate battery electrode materials, it is crucial to understand the ion intercalation and degradation mechanisms occurring during realistic battery operation. Here we apply a laboratory-based operando optical scattering microscopy method to study micrometre-sized rod-like particles of the anode material Nb14W3O44 during high-rate cycling. We directly visualize elongation of the particles, which, by comparison with ensemble X-ray diffraction, allows us to determine changes in the state of charge of individual particles. A continuous change in scattering intensity with state of charge enables the observation of non-equilibrium kinetic phase separations within individual particles. Phase field modelling (informed by pulsed-field-gradient nuclear magnetic resonance and electrochemical experiments) supports the kinetic origin of this separation, which arises from the state-of-charge dependence of the Li-ion diffusion coefficient. The non-equilibrium phase separations lead to particle cracking at high rates of delithiation, particularly in longer particles, with some of the resulting fragments becoming electrically disconnected on subsequent cycling. These results demonstrate the power of optical scattering microscopy to track rapid non-equilibrium processes that would be inaccessible with established characterization techniques.


These are the other notes that link to this one.

Nothing links here, how did you reach this page then?


Share your thoughts on this note
Aquiles Carattino
Aquiles Carattino
This note you are reading is part of my digital garden. Follow the links to learn more, and remember that these notes evolve over time. After all, this website is not a blog.
© 2021 Aquiles Carattino
This work is licensed under a Creative Commons Attribution-ShareAlike 4.0 International License
Privacy Policy