Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes

The sulfide solid electrolyte Li6PS5Cl has beenshown to be an ideal candidate for use in composite electrodes forall solid-state lithium-ion batteries due to its high ionicconductivity, low activation energy, and rapid processability insolvents (solution-based processing). Many reports for solution-...

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Autores: Warren, Zachary, Seghers, Miguel, Boissière, Pierre, Aparicio, Mario, Rosero-Navarro, Nataly Carolina
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/382205
Acceso en línea:http://hdl.handle.net/10261/382205
Access Level:acceso abierto
Palabra clave:solid electrolytes
Li6PS5Cl
argyrodite
sintering
solution-based synthesis.
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spelling Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite ElectrodesWarren, ZacharySeghers, MiguelBoissière, PierreAparicio, MarioRosero-Navarro, Nataly Carolinasolid electrolytesLi6PS5Clargyroditesinteringsolution-based synthesis.The sulfide solid electrolyte Li6PS5Cl has beenshown to be an ideal candidate for use in composite electrodes forall solid-state lithium-ion batteries due to its high ionicconductivity, low activation energy, and rapid processability insolvents (solution-based processing). Many reports for solution-based processing of Li6PS5Cl required the electrolyte to bedensified or sealed inside of a closed-quartz vessel prior to a finalhigh-temperature sintering step. This pre-sintering step is useful forunderstanding the full electrochemical properties of the electrolytebut provides little information about usable electrolyte powders forcommercialization. Modern applications of solid electrolytepowders require a feedstock of powdered electrolyte, which canbe processed by tape-casting, screen-printing, aerosol deposition,electrophoretic deposition, and hot powder rolling. The lack of information regarding the sintering of Li6PS5Cl powders for bulkprocessing warrants an investigation into open vessel sintering of solely the Li6PS5Cl electrolyte powders, which can later be used incomposite electrodes. This research uses a solution-based processing technique to synthesize Li6PS5Cl prior to sintering in open-topborosilicate glass containers. Here we show the effects that sintering temperatures have on Li6PS5Cl electrolyte powders duringopen-vessel sintering using X-ray diffraction, scanning electron microscopy, and Raman spectroscopy for morphological analysis.Electrochemical characterization was performed using AC electrical impedance spectroscopy, cyclic voltammetry, andchronoamperometry. Lastly, a full solid-state electrochemical cell was constructed with a cathode composite electrode madefrom the Li6PS5Cl to illustrate the functionality of the electrolyte.This research work is part of PIE project “Innovative andDesigned (Electro)-Chemistry, All-in-One for Lithium SulfideSolid Electrolytes” (IDEAL-Li), reference 20226AT009supported by The Spanish National Research Council(CSIC). Financial support of this work through Ramon yCajal Grant No. RYC2020−029909-I of The Spanish StateResearch Agency to N.C. Rosero-Navarro. Partially supportedby Microxide Project of The Spanish State Research Agency,TED2021−130911B−I00, funded by MCIN/AEI/10.13039/501100011033, and by the European Union “NextGener-ationEU”/PRT. Pierre Boissiè re thanks Erasmus+ Programmefor supporting educational training internship, agreement174191-2023Peer reviewedAmerican Chemical SocietyConsejo Superior de Investigaciones Científicas (España)Agencia Estatal de Investigación (España)European CommissionConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252025info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/382205reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI//RYC2020−029909-Iinfo:eu-repo/grantAgreement/AEI//TED2021-130911B-I00info:eu-repo/grantAgreement/EC//174191https://doi.org/10.1021/acselectrochem.4c00228Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3822052026-05-22T06:33:51Z
dc.title.none.fl_str_mv Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
title Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
spellingShingle Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
Warren, Zachary
solid electrolytes
Li6PS5Cl
argyrodite
sintering
solution-based synthesis.
title_short Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
title_full Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
title_fullStr Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
title_full_unstemmed Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
title_sort Effect of Temperature during Open Vessel Sintering on Li6PS5Cl Solid-State Electrolyte Powders for Use in Cathode Composite Electrodes
dc.creator.none.fl_str_mv Warren, Zachary
Seghers, Miguel
Boissière, Pierre
Aparicio, Mario
Rosero-Navarro, Nataly Carolina
author Warren, Zachary
author_facet Warren, Zachary
Seghers, Miguel
Boissière, Pierre
Aparicio, Mario
Rosero-Navarro, Nataly Carolina
author_role author
author2 Seghers, Miguel
Boissière, Pierre
Aparicio, Mario
Rosero-Navarro, Nataly Carolina
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Consejo Superior de Investigaciones Científicas (España)
Agencia Estatal de Investigación (España)
European Commission
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv solid electrolytes
Li6PS5Cl
argyrodite
sintering
solution-based synthesis.
topic solid electrolytes
Li6PS5Cl
argyrodite
sintering
solution-based synthesis.
description The sulfide solid electrolyte Li6PS5Cl has beenshown to be an ideal candidate for use in composite electrodes forall solid-state lithium-ion batteries due to its high ionicconductivity, low activation energy, and rapid processability insolvents (solution-based processing). Many reports for solution-based processing of Li6PS5Cl required the electrolyte to bedensified or sealed inside of a closed-quartz vessel prior to a finalhigh-temperature sintering step. This pre-sintering step is useful forunderstanding the full electrochemical properties of the electrolytebut provides little information about usable electrolyte powders forcommercialization. Modern applications of solid electrolytepowders require a feedstock of powdered electrolyte, which canbe processed by tape-casting, screen-printing, aerosol deposition,electrophoretic deposition, and hot powder rolling. The lack of information regarding the sintering of Li6PS5Cl powders for bulkprocessing warrants an investigation into open vessel sintering of solely the Li6PS5Cl electrolyte powders, which can later be used incomposite electrodes. This research uses a solution-based processing technique to synthesize Li6PS5Cl prior to sintering in open-topborosilicate glass containers. Here we show the effects that sintering temperatures have on Li6PS5Cl electrolyte powders duringopen-vessel sintering using X-ray diffraction, scanning electron microscopy, and Raman spectroscopy for morphological analysis.Electrochemical characterization was performed using AC electrical impedance spectroscopy, cyclic voltammetry, andchronoamperometry. Lastly, a full solid-state electrochemical cell was constructed with a cathode composite electrode madefrom the Li6PS5Cl to illustrate the functionality of the electrolyte.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/382205
url http://hdl.handle.net/10261/382205
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/AEI//RYC2020−029909-I
info:eu-repo/grantAgreement/AEI//TED2021-130911B-I00
info:eu-repo/grantAgreement/EC//174191
https://doi.org/10.1021/acselectrochem.4c00228

dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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