Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ charact...

Autores
Da Silva, Débora A. C.; Pinzón, Manuel J.; Messias Da Silva, Andresa; Fileti, Eudes E.; Pascon, Aline; Franco, Débora V.; Da Silva, Leonardo Morais; Zanin, Hudson G.
Año de publicación
2022
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We report here molecular dynamics simulations combined with in situ experimental studies to understand the advantages and disadvantages of replacing conventional (salt-in-water, SiWE) aqueous-based electrolytes with very concentrated (water-in-salt, WiSE) systems in supercapacitors. Atomistic molecular dynamics simulations were employed to investigate the energetic, structural, and transport properties of aqueous electrolytes based on sodium perchlorate (NaClO4). Simulations covered the concentrations range of 1 mol dm-3 (1 mol kg-1) to 8 mol dm-3 (15 mol kg-1), demonstrating a significant increase in viscosity and density and reduction in ionic conductivity as the concentration reaches the WiSE conditions. A carbon-based symmetric supercapacitor filled with WiSE showed a larger electrochemical stability window (ESW), allowing to span the cell voltage and specific energy. Larger ESW values are possible due to the formation of a solvent blocking interface (SBI). The formation of ionic aggregates owing to the increasing cohesive energy in WiSE disturbs the hydrogen-bond network resulting in physicochemical changes in the bulk liquid phase. In addition, the molal ratio between water and ions is decreased, resulting in a low interaction of the water molecules with the electrode at the interface, thus inhibiting the water-splitting considerably.
Fil: Da Silva, Débora A. C.. Universidade Estadual de Campinas; Brasil
Fil: Pinzón, Manuel J.. Universidade Estadual de Campinas; Brasil
Fil: Messias Da Silva, Andresa. Universidad Federal do Abc; Brasil. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Fileti, Eudes E.. Universidade de Sao Paulo; Brasil
Fil: Pascon, Aline. Universidade Estadual de Campinas; Brasil
Fil: Franco, Débora V.. University of Jequitinhonha e Mucuri's Valley; Brasil
Fil: Da Silva, Leonardo Morais. University of Jequitinhonha e Mucuri's Valley; Brasil
Fil: Zanin, Hudson G.. Universidade Estadual de Campinas; Brasil
Materia
electrolytes
energy storage
supercapacitor
water-in-salt
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/214480
Acceder
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network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studiesDa Silva, Débora A. C.Pinzón, Manuel J.Messias Da Silva, AndresaFileti, Eudes E.Pascon, AlineFranco, Débora V.Da Silva, Leonardo MoraisZanin, Hudson G.electrolytesenergy storagesupercapacitorwater-in-salthttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We report here molecular dynamics simulations combined with in situ experimental studies to understand the advantages and disadvantages of replacing conventional (salt-in-water, SiWE) aqueous-based electrolytes with very concentrated (water-in-salt, WiSE) systems in supercapacitors. Atomistic molecular dynamics simulations were employed to investigate the energetic, structural, and transport properties of aqueous electrolytes based on sodium perchlorate (NaClO4). Simulations covered the concentrations range of 1 mol dm-3 (1 mol kg-1) to 8 mol dm-3 (15 mol kg-1), demonstrating a significant increase in viscosity and density and reduction in ionic conductivity as the concentration reaches the WiSE conditions. A carbon-based symmetric supercapacitor filled with WiSE showed a larger electrochemical stability window (ESW), allowing to span the cell voltage and specific energy. Larger ESW values are possible due to the formation of a solvent blocking interface (SBI). The formation of ionic aggregates owing to the increasing cohesive energy in WiSE disturbs the hydrogen-bond network resulting in physicochemical changes in the bulk liquid phase. In addition, the molal ratio between water and ions is decreased, resulting in a low interaction of the water molecules with the electrode at the interface, thus inhibiting the water-splitting considerably.Fil: Da Silva, Débora A. C.. Universidade Estadual de Campinas; BrasilFil: Pinzón, Manuel J.. Universidade Estadual de Campinas; BrasilFil: Messias Da Silva, Andresa. Universidad Federal do Abc; Brasil. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Fileti, Eudes E.. Universidade de Sao Paulo; BrasilFil: Pascon, Aline. Universidade Estadual de Campinas; BrasilFil: Franco, Débora V.. University of Jequitinhonha e Mucuri's Valley; BrasilFil: Da Silva, Leonardo Morais. University of Jequitinhonha e Mucuri's Valley; BrasilFil: Zanin, Hudson G.. Universidade Estadual de Campinas; BrasilRoyal Society of Chemistry2022-01info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/214480Da Silva, Débora A. C.; Pinzón, Manuel J.; Messias Da Silva, Andresa; Fileti, Eudes E.; Pascon, Aline; et al.; Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies; Royal Society of Chemistry; Materials Advances; 3; 1; 1-2022; 611-6232633-5409CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1039/d1ma00890kinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:27:44Zoai:ri.conicet.gov.ar:11336/214480instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-15 14:27:44.528CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
title Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
spellingShingle Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
Da Silva, Débora A. C.
electrolytes
energy storage
supercapacitor
water-in-salt
title_short Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
title_full Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
title_fullStr Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
title_full_unstemmed Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
title_sort Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies
dc.creator.none.fl_str_mv Da Silva, Débora A. C.
Pinzón, Manuel J.
Messias Da Silva, Andresa
Fileti, Eudes E.
Pascon, Aline
Franco, Débora V.
Da Silva, Leonardo Morais
Zanin, Hudson G.
author Da Silva, Débora A. C.
author_facet Da Silva, Débora A. C.
Pinzón, Manuel J.
Messias Da Silva, Andresa
Fileti, Eudes E.
Pascon, Aline
Franco, Débora V.
Da Silva, Leonardo Morais
Zanin, Hudson G.
author_role author
author2 Pinzón, Manuel J.
Messias Da Silva, Andresa
Fileti, Eudes E.
Pascon, Aline
Franco, Débora V.
Da Silva, Leonardo Morais
Zanin, Hudson G.
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv electrolytes
energy storage
supercapacitor
water-in-salt
topic electrolytes
energy storage
supercapacitor
water-in-salt
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv We report here molecular dynamics simulations combined with in situ experimental studies to understand the advantages and disadvantages of replacing conventional (salt-in-water, SiWE) aqueous-based electrolytes with very concentrated (water-in-salt, WiSE) systems in supercapacitors. Atomistic molecular dynamics simulations were employed to investigate the energetic, structural, and transport properties of aqueous electrolytes based on sodium perchlorate (NaClO4). Simulations covered the concentrations range of 1 mol dm-3 (1 mol kg-1) to 8 mol dm-3 (15 mol kg-1), demonstrating a significant increase in viscosity and density and reduction in ionic conductivity as the concentration reaches the WiSE conditions. A carbon-based symmetric supercapacitor filled with WiSE showed a larger electrochemical stability window (ESW), allowing to span the cell voltage and specific energy. Larger ESW values are possible due to the formation of a solvent blocking interface (SBI). The formation of ionic aggregates owing to the increasing cohesive energy in WiSE disturbs the hydrogen-bond network resulting in physicochemical changes in the bulk liquid phase. In addition, the molal ratio between water and ions is decreased, resulting in a low interaction of the water molecules with the electrode at the interface, thus inhibiting the water-splitting considerably.
Fil: Da Silva, Débora A. C.. Universidade Estadual de Campinas; Brasil
Fil: Pinzón, Manuel J.. Universidade Estadual de Campinas; Brasil
Fil: Messias Da Silva, Andresa. Universidad Federal do Abc; Brasil. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Fileti, Eudes E.. Universidade de Sao Paulo; Brasil
Fil: Pascon, Aline. Universidade Estadual de Campinas; Brasil
Fil: Franco, Débora V.. University of Jequitinhonha e Mucuri's Valley; Brasil
Fil: Da Silva, Leonardo Morais. University of Jequitinhonha e Mucuri's Valley; Brasil
Fil: Zanin, Hudson G.. Universidade Estadual de Campinas; Brasil
description We report here molecular dynamics simulations combined with in situ experimental studies to understand the advantages and disadvantages of replacing conventional (salt-in-water, SiWE) aqueous-based electrolytes with very concentrated (water-in-salt, WiSE) systems in supercapacitors. Atomistic molecular dynamics simulations were employed to investigate the energetic, structural, and transport properties of aqueous electrolytes based on sodium perchlorate (NaClO4). Simulations covered the concentrations range of 1 mol dm-3 (1 mol kg-1) to 8 mol dm-3 (15 mol kg-1), demonstrating a significant increase in viscosity and density and reduction in ionic conductivity as the concentration reaches the WiSE conditions. A carbon-based symmetric supercapacitor filled with WiSE showed a larger electrochemical stability window (ESW), allowing to span the cell voltage and specific energy. Larger ESW values are possible due to the formation of a solvent blocking interface (SBI). The formation of ionic aggregates owing to the increasing cohesive energy in WiSE disturbs the hydrogen-bond network resulting in physicochemical changes in the bulk liquid phase. In addition, the molal ratio between water and ions is decreased, resulting in a low interaction of the water molecules with the electrode at the interface, thus inhibiting the water-splitting considerably.
publishDate 2022
dc.date.none.fl_str_mv 2022-01
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/214480
Da Silva, Débora A. C.; Pinzón, Manuel J.; Messias Da Silva, Andresa; Fileti, Eudes E.; Pascon, Aline; et al.; Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies; Royal Society of Chemistry; Materials Advances; 3; 1; 1-2022; 611-623
2633-5409
CONICET Digital
CONICET
url http://hdl.handle.net/11336/214480
identifier_str_mv Da Silva, Débora A. C.; Pinzón, Manuel J.; Messias Da Silva, Andresa; Fileti, Eudes E.; Pascon, Aline; et al.; Effect of conductivity, viscosity, and density of water-in-salt electrolytes on the electrochemical behavior of supercapacitors: Molecular dynamics simulations and: In situ characterization studies; Royal Society of Chemistry; Materials Advances; 3; 1; 1-2022; 611-623
2633-5409
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1039/d1ma00890k
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1846082735418900480
score 13.22299

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