NASICON LiM2(PO4)3 electrolyte (M = Zr) and electrode (M = Ti) materials for all solid-state Li-ion batteries with high total conductivity and low interfacial resistance

El-Shinawi, H., Regoutz, A., Payne, D. J., Cussen, E. J. and Corr, S. A. (2018) NASICON LiM2(PO4)3 electrolyte (M = Zr) and electrode (M = Ti) materials for all solid-state Li-ion batteries with high total conductivity and low interfacial resistance. Journal of Materials Chemistry A, 6(13), pp. 5296-5303. (doi: 10.1039/C7TA08715B)

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Abstract

All solid-state batteries based on NASICON-type LiM2(PO4)3 electrolyte phases are highly promising owing to their high ionic conductivities and chemical stabilities. Unlike Ti-based phases, extensively studied as Li+ solid electrolyte membranes, LiZr2(PO4)3 (LZP) is expected to form a stable interface with a metallic lithium anode, a challenge which has posed a serious roadblock to realising safe all solid-state batteries. However, prohibitively large grain boundary resistances are often observed in this material and this issue, combined with processing difficulties in fabricating LZP in dense forms, has impinged on the application of LZP as a solid electrolyte for all solid-state batteries. To overcome these shortcomings and demonstrate the excellent potential of LZP as a solid electrolyte, we have developed a simple approach, based on sol–gel chemistry, to effectively improve the densification of the material leading to higher total conductivity than previously reported (1.0 × 10−4 S cm−1 at 80 °C) and enabling the investigation of the material as a Li+ solid electrolyte without the need for elaborate post-processing steps. The interfacial resistance decreases dramatically on using thin layers of Au buffer to improve the contact between Li and the LZP surface. The Li/LZP interface shows constant resistance upon Li+ cycling (at 40 μA cm−2), despite the formation of a passivation layer of Li3P/Li8ZrO6 on the LZP surface. This is consistent with the prediction that this surface layer serves as a Li+ conductive, solid electrolyte interface between Li and LZP. Finally, an analogue material, LiTi2(PO4)3, is also introduced and demonstrated as an electrode material for proposed LZP-based all-solid-state batteries.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Corr, Professor Serena and El-Shinawi, Dr Hany
Authors: El-Shinawi, H., Regoutz, A., Payne, D. 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
Published Online:23 January 2018
Copyright Holders:Copyright © 2018 The Royal Society of Chemistry
First Published:First published in Journal of Materials Chemistry A 6(13): 5296-5303
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
693531High throughput microwave synthesis of Li-ion battery materialsSerena CorrEngineering and Physical Sciences Research Council (EPSRC)EP/N001982/1SCHOOL OF CHEMISTRY