Dendrite nucleation in lithium-conductive ceramics

Li, G. and Monroe, C. W. (2019) Dendrite nucleation in lithium-conductive ceramics. Physical Chemistry Chemical Physics, 21(36), pp. 20354-20359. (doi: 10.1039/C9CP03884A) (PMID:31497811)

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Solid-state lithium batteries cannot achieve reasonable power densities because of dendrites, whose formation mechanisms remain uncertain. This paper applies principles of chemomechanics to investigate the critical current above which dendrites form in lithium-conductive ceramics. Applied voltage induces stress in solid electrolytes; dendrites appear to nucleate in the exemplary garnet-oxide material Li7La3Zr2O12 (LLZO) when the interfacial pressure exceeds a particular value. The critical pressure of polycrystalline LLZO correlates well with the surface-energy changes incurred by lithium plating in its grain boundaries. A derived formula, validated by experiments, predicts quantitatively how critical current varies with properties including interfacial impedance, bulk permittivity, and grain size. As well as suggesting novel strategies to create more resilient ion-conductive ceramics, the proposed mechanism rationalizes experimental observations of bulk lithium plating and explains how LLZO exhibits an electrically activated transition from stable low-current cyclability to high-current dendrite nucleation.

Item Type:Articles
Additional Information:This work was supported by the Faraday Institution SOLBAT challenge, grant no. FIRG007, and the Engineering and Physical Sciences Research Council (EPSRC), grant no. EP/P003532/1.
Glasgow Author(s) Enlighten ID:Li, Dr Guanchen
Authors: Li, G., and Monroe, C. W.
College/School:College of Science and Engineering > School of Engineering > Systems Power and Energy
Journal Name:Physical Chemistry Chemical Physics
Publisher:Royal Society of Chemistry
ISSN (Online):1463-9084
Published Online:09 September 2019
Copyright Holders:Copyright © 2019 The Owner Societies
First Published:First published in Physical Chemistry Chemical Physics 21(36): 20354-20359
Publisher Policy:Reproduced under a Creative Commons License

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