Fast microwave-assisted synthesis of Li-stuffed garnets and insights into Li diffusion from muon spin spectroscopy

Amores Segura, M., Ahston, T. E., Baker, P. J., Cussen, E. J. and Corr, S. A. (2016) Fast microwave-assisted synthesis of Li-stuffed garnets and insights into Li diffusion from muon spin spectroscopy. Journal of Materials Chemistry A, 4, pp. 1729-1736. (doi:10.1039/c5ta08107f)

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Abstract

Lithium-stuffed garnets attract huge attention due to their outstanding potential as solid-state electrolytes for lithium batteries. However, there exists a persistent challenge in the reliable synthesis of these complex functional oxides together with a lack of complete understanding of the lithium-ion diffusion mechanisms in these important materials. Addressing these issues is critical to realizing the application of garnet materials as electrolytes in all solid-state lithium-ion batteries. In this work, a cubic phase garnet of nominal composition Li6.5Al0.25La2.92Zr2O12 is synthesized through a microwave-assisted solid-state route for the first time, reducing considerably the reaction times and heating temperatures. Lithium-ion diffusion behavior is investigated by electrochemical impedance spectroscopy (EIS) and state-of-art muon spin relaxation (μSR) spectroscopy, displaying activation energies of 0.55 ± 0.03 eV and 0.19 ± 0.01 eV respectively. This difference arises from the high inter-grain resistance, which contributes to the total resistance in EIS measurements. In contrast, μSR acts as a local probe providing insights on the order of the lattice, giving an estimated value of 4.62 × 10−11 cm2 s−1 for the lithium diffusion coefficient. These results demonstrate the potential of this lithium-stuffed garnet as a solid-state electrolyte for all-solid state lithium-ion batteries, an area of growing interest in the energy storage community.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Corr, Professor Serena and Amores Segura, Mr Marco
Authors: Amores Segura, M., Ahston, T. E., Baker, P. J., Cussen, E. J., and Corr, S. A.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Journal of Materials Chemistry A
Publisher:Royal Society of Chemistry
ISSN:2050-7488
ISSN (Online):2050-7496
Copyright Holders:Copyright © 2015 Royal Society of Chemistry
First Published:First published in Journal of Materials Chemistry A 4:1729-1736
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
643201Microwave processing for fast, green preparation of insertion electrodesSerena CorrEngineering & Physical Sciences Research Council (EPSRC)EP/K029290/1SCHOOL OF CHEMISTRY
693531High throughput microwave synthesis of Li-ion battery materialsSerena CorrEngineering & Physical Sciences Research Council (EPSRC)EP/N001982/1SCHOOL OF CHEMISTRY