A stochastic exploration of the quantum conformational spaces in the microsolvation of divalent cations with explicit consideration of up to six solvent molecules [Mg (H 2 O) n )]2+, (n = 3, 4, 5, 6) at the B3LYP, MP2, CCSD(T) levels is presented. We find several cases in which the formal charge in...

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Fecha de publicación:
2013
Institución:
Universidad de Medellín
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Repositorio UDEM
Idioma:
eng
OAI Identifier:
oai:repository.udem.edu.co:11407/1356
Acceso en línea:
http://hdl.handle.net/11407/1356
Palabra clave:
Hydrogen bonding
Microsolvation of cations
Stochastic optimization
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spelling 2015-10-09T13:17:51Z2015-10-09T13:17:51Z201316102940http://hdl.handle.net/11407/135610.1007/s00894-012-1716-5A stochastic exploration of the quantum conformational spaces in the microsolvation of divalent cations with explicit consideration of up to six solvent molecules [Mg (H 2 O) n )]2+, (n = 3, 4, 5, 6) at the B3LYP, MP2, CCSD(T) levels is presented. We find several cases in which the formal charge in Mg2+ causes dissociation of water molecules in the first solvation shell, leaving a hydroxide ion available to interact with the central cation, the released proton being transferred to outer solvation shells in a Grotthus type mechanism; this particular finding sheds light on the capacity of Mg2+ to promote formation of hydroxide anions, a process necessary to regulate proton transfer in enzymes with exonuclease activity. Two distinct types of hydrogen bonds, scattered over a wide range of distances (1.35–2.15 Å) were identified. We find that in inner solvation shells, where hydrogen bond networks are severely disturbed, most of the interaction energies come from electrostatic and polarization+charge transfer, while in outer solvation shells the situation approximates that of pure water clusters.enghttp://link.springer.com/article/10.1007/s00894-012-1716-5#page-1Journal of Molecular Modeling, abril de 2013, volume 19, issue 4, pp 1763-1777ScopusArticleinfo:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501http://purl.org/coar/resource_type/c_2df8fbb1info:eu-repo/semantics/restrictedAccesshttp://purl.org/coar/access_right/c_16ecInstituto de Química, Universidad de Antioquia, AA 1226, Medellín, ColombiaDepartamento de Ciencias Básicas, Universidad de Medellín, Medellín, ColombiaDepartamento de Química, Universidad Nacional de Colombia, Av. Cra. 30 #45-03, Bogota, ColombiaGonzalez J.D.Florez E.Romero J.Reyes A.Restrepo A.Hydrogen bondingMicrosolvation of cationsStochastic optimizationMicrosolvation of Mg2+, Ca2+: Strong influence of formal charges in hydrogen bond networks11407/1356oai:repository.udem.edu.co:11407/13562020-05-27 18:30:16.603Repositorio Institucional Universidad de Medellinrepositorio@udem.edu.co
dc.title.english.eng.fl_str_mv Microsolvation of Mg2+, Ca2+: Strong influence of formal charges in hydrogen bond networks
dc.contributor.affiliation.spa.fl_str_mv Instituto de Química, Universidad de Antioquia, AA 1226, Medellín, Colombia
Departamento de Ciencias Básicas, Universidad de Medellín, Medellín, Colombia
Departamento de Química, Universidad Nacional de Colombia, Av. Cra. 30 #45-03, Bogota, Colombia
dc.subject.keyword.eng.fl_str_mv Hydrogen bonding
Microsolvation of cations
Stochastic optimization
topic Hydrogen bonding
Microsolvation of cations
Stochastic optimization
spellingShingle Hydrogen bonding
Microsolvation of cations
Stochastic optimization
description A stochastic exploration of the quantum conformational spaces in the microsolvation of divalent cations with explicit consideration of up to six solvent molecules [Mg (H 2 O) n )]2+, (n = 3, 4, 5, 6) at the B3LYP, MP2, CCSD(T) levels is presented. We find several cases in which the formal charge in Mg2+ causes dissociation of water molecules in the first solvation shell, leaving a hydroxide ion available to interact with the central cation, the released proton being transferred to outer solvation shells in a Grotthus type mechanism; this particular finding sheds light on the capacity of Mg2+ to promote formation of hydroxide anions, a process necessary to regulate proton transfer in enzymes with exonuclease activity. Two distinct types of hydrogen bonds, scattered over a wide range of distances (1.35–2.15 Å) were identified. We find that in inner solvation shells, where hydrogen bond networks are severely disturbed, most of the interaction energies come from electrostatic and polarization+charge transfer, while in outer solvation shells the situation approximates that of pure water clusters.
publishDate 2013
dc.date.created.none.fl_str_mv 2013
dc.date.accessioned.none.fl_str_mv 2015-10-09T13:17:51Z
dc.date.available.none.fl_str_mv 2015-10-09T13:17:51Z
dc.type.eng.fl_str_mv Article
dc.type.coar.fl_str_mv http://purl.org/coar/resource_type/c_6501
http://purl.org/coar/resource_type/c_2df8fbb1
dc.type.driver.none.fl_str_mv info:eu-repo/semantics/article
dc.identifier.issn.none.fl_str_mv 16102940
dc.identifier.uri.none.fl_str_mv http://hdl.handle.net/11407/1356
dc.identifier.doi.none.fl_str_mv 10.1007/s00894-012-1716-5
identifier_str_mv 16102940
10.1007/s00894-012-1716-5
url http://hdl.handle.net/11407/1356
dc.language.iso.none.fl_str_mv eng
language eng
dc.relation.isversionof.spa.fl_str_mv http://link.springer.com/article/10.1007/s00894-012-1716-5#page-1
dc.relation.ispartofen.eng.fl_str_mv Journal of Molecular Modeling, abril de 2013, volume 19, issue 4, pp 1763-1777
dc.rights.coar.fl_str_mv http://purl.org/coar/access_right/c_16ec
dc.rights.accessrights.none.fl_str_mv info:eu-repo/semantics/restrictedAccess
eu_rights_str_mv restrictedAccess
rights_invalid_str_mv http://purl.org/coar/access_right/c_16ec
dc.source.spa.fl_str_mv Scopus
institution Universidad de Medellín
repository.name.fl_str_mv Repositorio Institucional Universidad de Medellin
repository.mail.fl_str_mv repositorio@udem.edu.co
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