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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/214480
Ver los metadatos del registro completo
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CONICET Digital (CONICET) |
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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 Técnicas2025-09-29T09:38:32Zoai: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:34982025-09-29 09:38:32.598CONICET 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 |
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1844613218317631488 |
score |
13.070432 |