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...
- Autores:
- Tipo de recurso:
- Fecha de publicación:
- 2013
- Institución:
- Universidad de Medellín
- Repositorio:
- 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
- Rights
- restrictedAccess
- License
- http://purl.org/coar/access_right/c_16ec
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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 |
_version_ |
1814159219335626752 |