Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers

Solid-state batteries (SSBs) using lithium (Li) metal anodes and solid-state electrolytes (SSEs) can offer both improved energy densities and, by removing flammable liquid electrolytes, improved safety. The argyrodite-type Li6PS5Cl ceramic is an attractive candidate SSE material because of its high...

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Main Authors: Su, J, Pasta, M, Ning, Z, Gao, X, Bruce, PG, Grovenor, CRM
Format: Journal article
Language:English
Published: Royal Society of Chemistry 2022
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author Su, J
Pasta, M
Ning, Z
Gao, X
Bruce, PG
Grovenor, CRM
author_facet Su, J
Pasta, M
Ning, Z
Gao, X
Bruce, PG
Grovenor, CRM
author_sort Su, J
collection OXFORD
description Solid-state batteries (SSBs) using lithium (Li) metal anodes and solid-state electrolytes (SSEs) can offer both improved energy densities and, by removing flammable liquid electrolytes, improved safety. The argyrodite-type Li6PS5Cl ceramic is an attractive candidate SSE material because of its high ionic conductivity (>1 mS cm−1) at room temperature and relatively ductile mechanical properties. However, interface contact issues between the SSE and Li metal hamper the practical development of solid-state Li metal batteries. In this work, we show that the interfacial resistance between the Li6PS5Cl SSE and Li metal anode can be reduced to as low as 1.3 Ω cm2 in symmetric cells by introducing a thin amorphous and Li-ion conducting lithium phosphorus oxynitride (LiPON) interlayer. We demonstrate that this interlayer improves the wetting behaviour of the Li6PS5Cl SSE, and helps form an effective conformal interfacial contact between the Li6PS5Cl SSE and Li metal. LiPON coated Li6PS5Cl symmetric cells with reduced interfacial resistance exhibit stable Li plating/stripping cycling for over 1000 h at 0.5 mA cm−2, and a dramatically improved critical current density of 4.1 mA cm−2 at 30 °C. These results demonstrate a reliable thin-film coating strategy for improving contact between the SSEs and Li metal anodes, stabilizing interfaces and realizing the practical application of solid-state Li metal batteries.
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spelling oxford-uuid:e40d0210-4b82-4252-9c91-779a2ec02dfd2023-08-04T11:34:36ZInterfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayersJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:e40d0210-4b82-4252-9c91-779a2ec02dfdEnglishSymplectic ElementsRoyal Society of Chemistry2022Su, JPasta, MNing, ZGao, XBruce, PGGrovenor, CRMSolid-state batteries (SSBs) using lithium (Li) metal anodes and solid-state electrolytes (SSEs) can offer both improved energy densities and, by removing flammable liquid electrolytes, improved safety. The argyrodite-type Li6PS5Cl ceramic is an attractive candidate SSE material because of its high ionic conductivity (>1 mS cm−1) at room temperature and relatively ductile mechanical properties. However, interface contact issues between the SSE and Li metal hamper the practical development of solid-state Li metal batteries. In this work, we show that the interfacial resistance between the Li6PS5Cl SSE and Li metal anode can be reduced to as low as 1.3 Ω cm2 in symmetric cells by introducing a thin amorphous and Li-ion conducting lithium phosphorus oxynitride (LiPON) interlayer. We demonstrate that this interlayer improves the wetting behaviour of the Li6PS5Cl SSE, and helps form an effective conformal interfacial contact between the Li6PS5Cl SSE and Li metal. LiPON coated Li6PS5Cl symmetric cells with reduced interfacial resistance exhibit stable Li plating/stripping cycling for over 1000 h at 0.5 mA cm−2, and a dramatically improved critical current density of 4.1 mA cm−2 at 30 °C. These results demonstrate a reliable thin-film coating strategy for improving contact between the SSEs and Li metal anodes, stabilizing interfaces and realizing the practical application of solid-state Li metal batteries.
spellingShingle Su, J
Pasta, M
Ning, Z
Gao, X
Bruce, PG
Grovenor, CRM
Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title_full Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title_fullStr Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title_full_unstemmed Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title_short Interfacial modification between argyrodite-type solid-state electrolytes and Li metal anodes using LiPON interlayers
title_sort interfacial modification between argyrodite type solid state electrolytes and li metal anodes using lipon interlayers
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AT pastam interfacialmodificationbetweenargyroditetypesolidstateelectrolytesandlimetalanodesusingliponinterlayers
AT ningz interfacialmodificationbetweenargyroditetypesolidstateelectrolytesandlimetalanodesusingliponinterlayers
AT gaox interfacialmodificationbetweenargyroditetypesolidstateelectrolytesandlimetalanodesusingliponinterlayers
AT brucepg interfacialmodificationbetweenargyroditetypesolidstateelectrolytesandlimetalanodesusingliponinterlayers
AT grovenorcrm interfacialmodificationbetweenargyroditetypesolidstateelectrolytesandlimetalanodesusingliponinterlayers