Polar mixtures under nanoconfinement

Autores
Rodriguez, Javier; Elola, Maria Dolores; Laria, Daniel Hector
Año de publicación
2009
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We present results from molecular dynamics simulations describing structural and dynamical characteristics of equimolar mixtures of water and acetonitrile, confined between two silica walls separated at interplate distances of d = 0.6, 1, and 1.5 nm. Two different environments were investigated: a first one where wall-solvent dispersion forces prevail (hydrophobic confinement) and a second one in which the terminal O atoms at the silica surface are transformed into silanol groups (hydrophilic confinement). For the former case, we found that, at the shortest interplate distance examined, the confined region is devoid of water molecules. At an interplate distance of the order of 1 nm, water moves into the confined region, although, in all cases, there is a clear enhancement of the local concentration of acetonitrile in detriment of that of water. Within hydrophilic environments, we found clear distinctions between a layer of bound water lying in close contact with the silica substrates and a minority of confined water that occupies the inner liquid slab. The bound aqueous layer is fully coordinated to the silanol groups and exhibits minimal hydrogen bonding with the second solvation layer, which exclusively includes acetonitrile molecules. Dynamical characteristics of the solvent mixture are analyzed in terms of diffusive and rotational motions in both environments. Compared to bulk mixtures, we found significant retardations in all dynamical modes, with those ascribed to water molecules bound to the hydrophilic plates being the most dramatic.
Fil: Rodriguez, Javier. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Elola, Maria Dolores. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina
Fil: Laria, Daniel Hector. Comisión Nacional de Energía Atómica; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina. 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
Materia
Water-Acetonitrile Mixtures
Molecular-Dynamics Simulation
Phase Separation Phenomena
Binary-Liquid Mixtures
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/83783
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/83783
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Polar mixtures under nanoconfinementRodriguez, JavierElola, Maria DoloresLaria, Daniel HectorWater-Acetonitrile MixturesMolecular-Dynamics SimulationPhase Separation PhenomenaBinary-Liquid Mixtureshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We present results from molecular dynamics simulations describing structural and dynamical characteristics of equimolar mixtures of water and acetonitrile, confined between two silica walls separated at interplate distances of d = 0.6, 1, and 1.5 nm. Two different environments were investigated: a first one where wall-solvent dispersion forces prevail (hydrophobic confinement) and a second one in which the terminal O atoms at the silica surface are transformed into silanol groups (hydrophilic confinement). For the former case, we found that, at the shortest interplate distance examined, the confined region is devoid of water molecules. At an interplate distance of the order of 1 nm, water moves into the confined region, although, in all cases, there is a clear enhancement of the local concentration of acetonitrile in detriment of that of water. Within hydrophilic environments, we found clear distinctions between a layer of bound water lying in close contact with the silica substrates and a minority of confined water that occupies the inner liquid slab. The bound aqueous layer is fully coordinated to the silanol groups and exhibits minimal hydrogen bonding with the second solvation layer, which exclusively includes acetonitrile molecules. Dynamical characteristics of the solvent mixture are analyzed in terms of diffusive and rotational motions in both environments. Compared to bulk mixtures, we found significant retardations in all dynamical modes, with those ascribed to water molecules bound to the hydrophilic plates being the most dramatic.Fil: Rodriguez, Javier. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; ArgentinaFil: Elola, Maria Dolores. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; ArgentinaFil: Laria, Daniel Hector. Comisión Nacional de Energía Atómica; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina. 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; ArgentinaAmerican Chemical Society2009-09info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/83783Rodriguez, Javier; Elola, Maria Dolores; Laria, Daniel Hector; Polar mixtures under nanoconfinement; American Chemical Society; Journal of Physical Chemistry B; 113; 38; 9-2009; 12744-127491089-56471520-6106CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jp905920minfo:eu-repo/semantics/altIdentifier/doi/10.1021/jp905920minfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:16:38Zoai:ri.conicet.gov.ar:11336/83783instacron: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 10:16:39.263CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Polar mixtures under nanoconfinement
title Polar mixtures under nanoconfinement
spellingShingle Polar mixtures under nanoconfinement
Rodriguez, Javier
Water-Acetonitrile Mixtures
Molecular-Dynamics Simulation
Phase Separation Phenomena
Binary-Liquid Mixtures
title_short Polar mixtures under nanoconfinement
title_full Polar mixtures under nanoconfinement
title_fullStr Polar mixtures under nanoconfinement
title_full_unstemmed Polar mixtures under nanoconfinement
title_sort Polar mixtures under nanoconfinement
dc.creator.none.fl_str_mv Rodriguez, Javier
Elola, Maria Dolores
Laria, Daniel Hector
author Rodriguez, Javier
author_facet Rodriguez, Javier
Elola, Maria Dolores
Laria, Daniel Hector
author_role author
author2 Elola, Maria Dolores
Laria, Daniel Hector
author2_role author
author
dc.subject.none.fl_str_mv Water-Acetonitrile Mixtures
Molecular-Dynamics Simulation
Phase Separation Phenomena
Binary-Liquid Mixtures
topic Water-Acetonitrile Mixtures
Molecular-Dynamics Simulation
Phase Separation Phenomena
Binary-Liquid Mixtures
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 present results from molecular dynamics simulations describing structural and dynamical characteristics of equimolar mixtures of water and acetonitrile, confined between two silica walls separated at interplate distances of d = 0.6, 1, and 1.5 nm. Two different environments were investigated: a first one where wall-solvent dispersion forces prevail (hydrophobic confinement) and a second one in which the terminal O atoms at the silica surface are transformed into silanol groups (hydrophilic confinement). For the former case, we found that, at the shortest interplate distance examined, the confined region is devoid of water molecules. At an interplate distance of the order of 1 nm, water moves into the confined region, although, in all cases, there is a clear enhancement of the local concentration of acetonitrile in detriment of that of water. Within hydrophilic environments, we found clear distinctions between a layer of bound water lying in close contact with the silica substrates and a minority of confined water that occupies the inner liquid slab. The bound aqueous layer is fully coordinated to the silanol groups and exhibits minimal hydrogen bonding with the second solvation layer, which exclusively includes acetonitrile molecules. Dynamical characteristics of the solvent mixture are analyzed in terms of diffusive and rotational motions in both environments. Compared to bulk mixtures, we found significant retardations in all dynamical modes, with those ascribed to water molecules bound to the hydrophilic plates being the most dramatic.
Fil: Rodriguez, Javier. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Elola, Maria Dolores. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina
Fil: Laria, Daniel Hector. Comisión Nacional de Energía Atómica; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina. 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
description We present results from molecular dynamics simulations describing structural and dynamical characteristics of equimolar mixtures of water and acetonitrile, confined between two silica walls separated at interplate distances of d = 0.6, 1, and 1.5 nm. Two different environments were investigated: a first one where wall-solvent dispersion forces prevail (hydrophobic confinement) and a second one in which the terminal O atoms at the silica surface are transformed into silanol groups (hydrophilic confinement). For the former case, we found that, at the shortest interplate distance examined, the confined region is devoid of water molecules. At an interplate distance of the order of 1 nm, water moves into the confined region, although, in all cases, there is a clear enhancement of the local concentration of acetonitrile in detriment of that of water. Within hydrophilic environments, we found clear distinctions between a layer of bound water lying in close contact with the silica substrates and a minority of confined water that occupies the inner liquid slab. The bound aqueous layer is fully coordinated to the silanol groups and exhibits minimal hydrogen bonding with the second solvation layer, which exclusively includes acetonitrile molecules. Dynamical characteristics of the solvent mixture are analyzed in terms of diffusive and rotational motions in both environments. Compared to bulk mixtures, we found significant retardations in all dynamical modes, with those ascribed to water molecules bound to the hydrophilic plates being the most dramatic.
publishDate 2009
dc.date.none.fl_str_mv 2009-09
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/11336/83783
Rodriguez, Javier; Elola, Maria Dolores; Laria, Daniel Hector; Polar mixtures under nanoconfinement; American Chemical Society; Journal of Physical Chemistry B; 113; 38; 9-2009; 12744-12749
1089-5647
1520-6106
CONICET Digital
CONICET
url http://hdl.handle.net/11336/83783
identifier_str_mv Rodriguez, Javier; Elola, Maria Dolores; Laria, Daniel Hector; Polar mixtures under nanoconfinement; American Chemical Society; Journal of Physical Chemistry B; 113; 38; 9-2009; 12744-12749
1089-5647
1520-6106
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jp905920m
info:eu-repo/semantics/altIdentifier/doi/10.1021/jp905920m
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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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score 13.070432

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