Xie, W;
Deng, Z;
Liu, Z;
Famprikis, T;
Butler, KT;
Canepa, P;
(2024)
Effects of Grain Boundaries and Surfaces on Electronic and Mechanical Properties of Solid Electrolytes.
Advanced Energy Materials
, Article 2304230. 10.1002/aenm.202304230.
(In press).
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Abstract
Extended defects, including exposed surfaces and grain boundaries (GBs), are critical to the properties of polycrystalline solid electrolytes in all-solid-state batteries (ASSBs). These defects can alter the mechanical and electronic properties of solid electrolytes, with direct manifestations in the performance of ASSBs. Here, by building a library of 590 surfaces and grain boundaries of 11 relevant solid electrolytes—including halides, oxides, and sulfides— their electronic, mechanical, and thermodynamic characteristics are linked to the functional properties of polycrystalline solid electrolytes. It is found that the energy required to mechanically “separate” grain boundaries can be significantly lower than in the bulk region of materials, which can trigger preferential cracking of solid electrolyte particles in the grain boundary regions. The brittleness of ceramic solid electrolytes, inferred from the predicted low fracture toughness at the grain boundaries, contributes to their cracking under local pressure imparted by lithium (sodium) penetration in the grain boundaries. Extended defects of solid electrolytes introduce new electronic interfacial states within bandgaps of solid electrolytes. These states alter and possibly increase locally the availability of free electrons and holes in solid electrolytes. Factoring effects arising from extended defects appear crucial to explain electrochemical and mechanical observations in ASSBs.
| Type: | Article |
|---|---|
| Title: | Effects of Grain Boundaries and Surfaces on Electronic and Mechanical Properties of Solid Electrolytes |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/aenm.202304230 |
| Publisher version: | http://dx.doi.org/10.1002/aenm.202304230 |
| Language: | English |
| Additional information: | © 2024 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made. |
| Keywords: | Electronic properties, first-principles, calculations, grain boundaries, mechanical properties, solid electrolytes, surfaces |
| 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/10186449 |
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