QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water

Autores
González Lebrero, Mariano Camilo; Estrin, Dario Ariel
Año de publicación
2007
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We have investigated the reaction of peroxynitrite with carbon dioxide in aqueoussolution by means of combined quantum-classical (QM-MM) molecular dynamics simulations.In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussianbasis set, and the solvent was described using the mean-field TIP4P force field. The free energyprofile of this reaction has been computed using umbrella sampling and multiple steeringmolecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much moreefficient than MSMD schemes, due to the possibility of employing a combination of classicaland QM-MM thermalization schemes. We found the presence of a significant barrier in the freeenergy profile associated with the reaction in solution, which is not present in vacuum, that maybe ascribed to the significant charge redistribution upon reaction and the concomitant solvationpattern changes.
Fil: González Lebrero, Mariano Camilo. 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: Estrin, Dario Ariel. 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
peroxynitrite
QM-MM
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:11336/103155
Acceder
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network_name_str CONICET Digital (CONICET)
spelling QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in WaterGonzález Lebrero, Mariano CamiloEstrin, Dario ArielperoxynitriteQM-MMhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We have investigated the reaction of peroxynitrite with carbon dioxide in aqueoussolution by means of combined quantum-classical (QM-MM) molecular dynamics simulations.In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussianbasis set, and the solvent was described using the mean-field TIP4P force field. The free energyprofile of this reaction has been computed using umbrella sampling and multiple steeringmolecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much moreefficient than MSMD schemes, due to the possibility of employing a combination of classicaland QM-MM thermalization schemes. We found the presence of a significant barrier in the freeenergy profile associated with the reaction in solution, which is not present in vacuum, that maybe ascribed to the significant charge redistribution upon reaction and the concomitant solvationpattern changes.Fil: González Lebrero, Mariano Camilo. 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: Estrin, Dario Ariel. 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 Society2007-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/103155González Lebrero, Mariano Camilo; Estrin, Dario Ariel; QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water; American Chemical Society; Journal of Chemical Theory and Computation; 3; 4; 6-2007; 1405-14111549-9618CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/abs/10.1021/ct700038winfo:eu-repo/semantics/altIdentifier/doi/10.1021/ct700038winfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:43:22Zoai:ri.conicet.gov.ar:11336/103155instacron: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:34982025-09-03 09:43:22.555CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
title QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
spellingShingle QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
González Lebrero, Mariano Camilo
peroxynitrite
QM-MM
title_short QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
title_full QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
title_fullStr QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
title_full_unstemmed QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
title_sort QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water
dc.creator.none.fl_str_mv González Lebrero, Mariano Camilo
Estrin, Dario Ariel
author González Lebrero, Mariano Camilo
author_facet González Lebrero, Mariano Camilo
Estrin, Dario Ariel
author_role author
author2 Estrin, Dario Ariel
author2_role author
dc.subject.none.fl_str_mv peroxynitrite
QM-MM
topic peroxynitrite
QM-MM
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 have investigated the reaction of peroxynitrite with carbon dioxide in aqueoussolution by means of combined quantum-classical (QM-MM) molecular dynamics simulations.In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussianbasis set, and the solvent was described using the mean-field TIP4P force field. The free energyprofile of this reaction has been computed using umbrella sampling and multiple steeringmolecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much moreefficient than MSMD schemes, due to the possibility of employing a combination of classicaland QM-MM thermalization schemes. We found the presence of a significant barrier in the freeenergy profile associated with the reaction in solution, which is not present in vacuum, that maybe ascribed to the significant charge redistribution upon reaction and the concomitant solvationpattern changes.
Fil: González Lebrero, Mariano Camilo. 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: Estrin, Dario Ariel. 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 have investigated the reaction of peroxynitrite with carbon dioxide in aqueoussolution by means of combined quantum-classical (QM-MM) molecular dynamics simulations.In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussianbasis set, and the solvent was described using the mean-field TIP4P force field. The free energyprofile of this reaction has been computed using umbrella sampling and multiple steeringmolecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much moreefficient than MSMD schemes, due to the possibility of employing a combination of classicaland QM-MM thermalization schemes. We found the presence of a significant barrier in the freeenergy profile associated with the reaction in solution, which is not present in vacuum, that maybe ascribed to the significant charge redistribution upon reaction and the concomitant solvationpattern changes.
publishDate 2007
dc.date.none.fl_str_mv 2007-06
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/11336/103155
González Lebrero, Mariano Camilo; Estrin, Dario Ariel; QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water; American Chemical Society; Journal of Chemical Theory and Computation; 3; 4; 6-2007; 1405-1411
1549-9618
CONICET Digital
CONICET
url http://hdl.handle.net/11336/103155
identifier_str_mv González Lebrero, Mariano Camilo; Estrin, Dario Ariel; QM-MM Investigation of the Reaction of Peroxynitrite with Carbon Dioxide in Water; American Chemical Society; Journal of Chemical Theory and Computation; 3; 4; 6-2007; 1405-1411
1549-9618
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/abs/10.1021/ct700038w
info:eu-repo/semantics/altIdentifier/doi/10.1021/ct700038w
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
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 13.13397

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