Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures

Molecular dynamics simulations of sulfuric acid solutions at several temperatures (230, 250, 273 and 298 K) and concentrations (10, 20, 30 and 40 wt%) have been carried out. The dissociation of the acid has been explicitly considered, in accordance with the available experimental measurements. So, t...

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Detalles Bibliográficos
Autores: Canales Gabriel, Manel|||0000-0001-5503-8100, Guàrdia Manuel, Elvira|||0000-0002-4569-534X
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/362677
Acceso en línea:https://hdl.handle.net/2117/362677
https://dx.doi.org/10.1016/j.molliq.2021.118351
Access Level:acceso abierto
Palabra clave:Thermodynamics
Hydrogen
Aqueous sulfuric acid solutions
Molecular dynamics simulations
Viscosity and diffusion
Structural properties Hydrogen bond networks
Continuous and interrupted hydrogen bond lifetimes
Termodinàmica
Hidrogen
Àrees temàtiques de la UPC::Física::Termodinàmica
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spelling Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperaturesCanales Gabriel, Manel|||0000-0001-5503-8100Guàrdia Manuel, Elvira|||0000-0002-4569-534XThermodynamicsHydrogenAqueous sulfuric acid solutionsMolecular dynamics simulationsViscosity and diffusionStructural properties Hydrogen bond networksContinuous and interrupted hydrogen bond lifetimesTermodinàmicaHidrogenÀrees temàtiques de la UPC::Física::TermodinàmicaMolecular dynamics simulations of sulfuric acid solutions at several temperatures (230, 250, 273 and 298 K) and concentrations (10, 20, 30 and 40 wt%) have been carried out. The dissociation of the acid has been explicitly considered, in accordance with the available experimental measurements. So, the simulated systems are made up of the following molecular constituent species: water molecules, hydronium cations, bisulfate anions and sulfate dianions. Calculations have been conducted using a reliable force field, which allows us to determine density and viscosity values, which are in a reasonably good agreement with the available experimental data in the temperature and concentration ranges considered in this work. Simulations have also been employed to determine the radial distribution functions, which involve water molecules, and the diffusion coefficients of the constituent species. Moreover, a hydrogen bond analysis, involving only water molecules, has also been fulfilled. To this end, the mean number of hydrogen bonds between water molecules and between ions and water molecules, the percentages of molecular species hydrogen bonded with a given number of water molecules, and the continuous and interrupted lifetimes have been calculated. We observe that most properties are mainly sensitive to the concentration. We also notice that water molecules bonded to the anions are more labile than those bonded to other water molecules or to hydronium ions, the labilities increasing when the temperature rises. Moreover, the characteristic tetrahedral structure of water vanishes when the concentration or the temperatures increases. In the first case because water molecules tend to bond to a larger number of ions. In the second because the mean number of hydrogen bonds between water molecules and their lifetimes decrease. Finally, we also estimate the activation energies from the interrupted lifetimes, the viscosity and the diffusion coefficients. We note that these energies are very similar and they increase when the concentration rises.Peer Reviewed20222022-02-0120222022-02-21journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/362677https://dx.doi.org/10.1016/j.molliq.2021.118351reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 International (CC BY 4.0)https://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3626772026-05-27T15:37:01Z
dc.title.none.fl_str_mv Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
title Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
spellingShingle Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
Canales Gabriel, Manel|||0000-0001-5503-8100
Thermodynamics
Hydrogen
Aqueous sulfuric acid solutions
Molecular dynamics simulations
Viscosity and diffusion
Structural properties Hydrogen bond networks
Continuous and interrupted hydrogen bond lifetimes
Termodinàmica
Hidrogen
Àrees temàtiques de la UPC::Física::Termodinàmica
title_short Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
title_full Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
title_fullStr Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
title_full_unstemmed Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
title_sort Computer simulation study of ion-water and water-water hydrogen bonds in sulfuric acid solutions at low temperatures
dc.creator.none.fl_str_mv Canales Gabriel, Manel|||0000-0001-5503-8100
Guàrdia Manuel, Elvira|||0000-0002-4569-534X
author Canales Gabriel, Manel|||0000-0001-5503-8100
author_facet Canales Gabriel, Manel|||0000-0001-5503-8100
Guàrdia Manuel, Elvira|||0000-0002-4569-534X
author_role author
author2 Guàrdia Manuel, Elvira|||0000-0002-4569-534X
author2_role author
dc.subject.none.fl_str_mv Thermodynamics
Hydrogen
Aqueous sulfuric acid solutions
Molecular dynamics simulations
Viscosity and diffusion
Structural properties Hydrogen bond networks
Continuous and interrupted hydrogen bond lifetimes
Termodinàmica
Hidrogen
Àrees temàtiques de la UPC::Física::Termodinàmica
topic Thermodynamics
Hydrogen
Aqueous sulfuric acid solutions
Molecular dynamics simulations
Viscosity and diffusion
Structural properties Hydrogen bond networks
Continuous and interrupted hydrogen bond lifetimes
Termodinàmica
Hidrogen
Àrees temàtiques de la UPC::Física::Termodinàmica
description Molecular dynamics simulations of sulfuric acid solutions at several temperatures (230, 250, 273 and 298 K) and concentrations (10, 20, 30 and 40 wt%) have been carried out. The dissociation of the acid has been explicitly considered, in accordance with the available experimental measurements. So, the simulated systems are made up of the following molecular constituent species: water molecules, hydronium cations, bisulfate anions and sulfate dianions. Calculations have been conducted using a reliable force field, which allows us to determine density and viscosity values, which are in a reasonably good agreement with the available experimental data in the temperature and concentration ranges considered in this work. Simulations have also been employed to determine the radial distribution functions, which involve water molecules, and the diffusion coefficients of the constituent species. Moreover, a hydrogen bond analysis, involving only water molecules, has also been fulfilled. To this end, the mean number of hydrogen bonds between water molecules and between ions and water molecules, the percentages of molecular species hydrogen bonded with a given number of water molecules, and the continuous and interrupted lifetimes have been calculated. We observe that most properties are mainly sensitive to the concentration. We also notice that water molecules bonded to the anions are more labile than those bonded to other water molecules or to hydronium ions, the labilities increasing when the temperature rises. Moreover, the characteristic tetrahedral structure of water vanishes when the concentration or the temperatures increases. In the first case because water molecules tend to bond to a larger number of ions. In the second because the mean number of hydrogen bonds between water molecules and their lifetimes decrease. Finally, we also estimate the activation energies from the interrupted lifetimes, the viscosity and the diffusion coefficients. We note that these energies are very similar and they increase when the concentration rises.
publishDate 2022
dc.date.none.fl_str_mv 2022
2022-02-01
2022
2022-02-21
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
AM
http://purl.org/coar/version/c_ab4af688f83e57aa
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/362677
https://dx.doi.org/10.1016/j.molliq.2021.118351
url https://hdl.handle.net/2117/362677
https://dx.doi.org/10.1016/j.molliq.2021.118351
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International (CC BY 4.0)
https://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International (CC BY 4.0)
https://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
collection UPCommons. Portal del coneixement obert de la UPC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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