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Localized concentration reversal of lithium during intercalation into nanoparticles.

Published version
Peer-reviewed

Type

Article

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Abstract

Nanoparticulate electrodes, such as Li x FePO4, have unique advantages over their microparticulate counterparts for the applications in Li-ion batteries because of the shortened diffusion path and access to nonequilibrium routes for fast Li incorporation, thus radically boosting power density of the electrodes. However, how Li intercalation occurs locally in a single nanoparticle of such materials remains unresolved because real-time observation at such a fine scale is still lacking. We report visualization of local Li intercalation via solid-solution transformation in individual Li x FePO4 nanoparticles, enabled by probing sub-angstrom changes in the lattice spacing in situ. The real-time observation reveals inhomogeneous intercalation, accompanied with an unexpected reversal of Li concentration at the nanometer scale. The origin of the reversal phenomenon is elucidated through phase-field simulations, and it is attributed to the presence of structurally different regions that have distinct chemical potential functions. The findings from this study provide a new perspective on the local intercalation dynamics in battery electrodes.

Description

Keywords

40 Engineering, 4016 Materials Engineering, 34 Chemical Sciences, 3406 Physical Chemistry, Nanotechnology, Bioengineering

Journal Title

Sci Adv

Conference Name

Journal ISSN

2375-2548
2375-2548

Volume Title

4

Publisher

American Association for the Advancement of Science (AAAS)