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The origin of chemical inhomogeneity in garnet electrolytes and its impact on the electrochemical performance

Brugge, RH; Pesci, FM; Cavallaro, A; Sole, C; Isaacs, MA; Kerherve, G; Weatherup, RS; (2020) The origin of chemical inhomogeneity in garnet electrolytes and its impact on the electrochemical performance. Journal of Materials Chemistry A , 8 (28) pp. 14265-14276. 10.1039/d0ta04974c. Green open access

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Abstract

The interface between solid electrolytes and lithium metal electrodes determines the performance of an all-solid-state battery in terms of the ability to demand high power densities and prevent the formation of lithium dendrites. This interface depends strongly on the nature of the solid electrolyte surface in contact with the metallic anode. In the garnet electrolyte/Li system, most papers have focused on the role of current inhomogeneities induced by void formation in the Li metal electrode and the presence of insulating reaction layers following air exposure. However, extended defects in the solid electrolyte induced by chemical and/or structural inhomogeneities can also lead to uneven current distribution, impacting the performance of these systems. In this work, we use complementary surface analysis techniques with varying analysis depths to probe chemical distribution within grains and grain boundaries at the surface and in the bulk of garnet-type electrolytes to explain their electrochemical performance. We show that morphology, post-treatments and storage conditions can greatly affect the surface chemical distribution of grains and grain boundaries. These properties are important to understand since they will dictate the ionic and electronic transport near the interfacial zone between metal and electrolyte which is key to determining chemo-mechanical stability.

Type: Article
Title: The origin of chemical inhomogeneity in garnet electrolytes and its impact on the electrochemical performance
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d0ta04974c
Language: English
Additional information: © The Royal Society of Chemistry. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10118176
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