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Article: Elucidating solvent contributions to solution reactions with Ab initio QM/MM methods
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TitleElucidating solvent contributions to solution reactions with Ab initio QM/MM methods
 
AuthorsHu, H1
Yang, W2
 
Issue Date2010
 
PublisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journal/jpcbfk
 
CitationJournal Of Physical Chemistry B, 2010, v. 114 n. 8, p. 2755-2759 [How to Cite?]
DOI: http://dx.doi.org/10.1021/jp905886q
 
AbstractComputer simulations of reaction processes in solution in general rely on the definition of a reaction coordinate and the determination of the thermodynamic changes of the system along the reaction coordinate. The reaction coordinate often is constituted of characteristic geometrical properties of the reactive solute species, while the contributions of solvent molecules are implicitly included in the thermodynamics of the solute degrees of freedoms. However, solvent dynamics can provide the driving force for the reaction process, and in such cases explicit description of the solvent contribution in the free energy of the reaction process becomes necessary. We report here a method that can be used to analyze the solvent contributions to the reaction activation free energies from the combined QM/MM minimum free-energy path simulations. The method was applied to the self-exchange SN2 reaction of CH3Cl + Cl-, showing that the importance of solvent-solute interactions to the reaction process. The results were further discussed in the context of coupling between solvent and solute molecules in reaction processes. © 2010 American Chemical Society.
 
ISSN1520-6106
2013 Impact Factor: 3.377
2013 SCImago Journal Rankings: 1.575
 
DOIhttp://dx.doi.org/10.1021/jp905886q
 
ISI Accession Number IDWOS:000274842600025
Funding AgencyGrant Number
National Institutes of Health
HKU
Funding Information:

Financial support from the National Institutes of Health (to W.Y.) and HKU (seed funding to H.H.) is greatly appreciated.

 
ReferencesReferences in Scopus
 
DC FieldValue
dc.contributor.authorHu, H
 
dc.contributor.authorYang, W
 
dc.date.accessioned2011-03-21T08:58:20Z
 
dc.date.available2011-03-21T08:58:20Z
 
dc.date.issued2010
 
dc.description.abstractComputer simulations of reaction processes in solution in general rely on the definition of a reaction coordinate and the determination of the thermodynamic changes of the system along the reaction coordinate. The reaction coordinate often is constituted of characteristic geometrical properties of the reactive solute species, while the contributions of solvent molecules are implicitly included in the thermodynamics of the solute degrees of freedoms. However, solvent dynamics can provide the driving force for the reaction process, and in such cases explicit description of the solvent contribution in the free energy of the reaction process becomes necessary. We report here a method that can be used to analyze the solvent contributions to the reaction activation free energies from the combined QM/MM minimum free-energy path simulations. The method was applied to the self-exchange SN2 reaction of CH3Cl + Cl-, showing that the importance of solvent-solute interactions to the reaction process. The results were further discussed in the context of coupling between solvent and solute molecules in reaction processes. © 2010 American Chemical Society.
 
dc.description.natureLink_to_subscribed_fulltext
 
dc.identifier.citationJournal Of Physical Chemistry B, 2010, v. 114 n. 8, p. 2755-2759 [How to Cite?]
DOI: http://dx.doi.org/10.1021/jp905886q
 
dc.identifier.doihttp://dx.doi.org/10.1021/jp905886q
 
dc.identifier.eissn1520-5207
 
dc.identifier.epage2759
 
dc.identifier.hkuros176617
 
dc.identifier.isiWOS:000274842600025
Funding AgencyGrant Number
National Institutes of Health
HKU
Funding Information:

Financial support from the National Institutes of Health (to W.Y.) and HKU (seed funding to H.H.) is greatly appreciated.

 
dc.identifier.issn1520-6106
2013 Impact Factor: 3.377
2013 SCImago Journal Rankings: 1.575
 
dc.identifier.issue8
 
dc.identifier.openurl
 
dc.identifier.pmid20121225
 
dc.identifier.scopuseid_2-s2.0-77749279961
 
dc.identifier.spage2755
 
dc.identifier.urihttp://hdl.handle.net/10722/132168
 
dc.identifier.volume114
 
dc.languageeng
 
dc.publisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journal/jpcbfk
 
dc.publisher.placeUnited States
 
dc.relation.ispartofJournal of Physical Chemistry B
 
dc.relation.referencesReferences in Scopus
 
dc.subject.meshCatalysis
 
dc.subject.meshComputer Simulation
 
dc.subject.meshEnzymes - chemistry - metabolism
 
dc.subject.meshProtein Conformation
 
dc.subject.meshQuantum Theory
 
dc.titleElucidating solvent contributions to solution reactions with Ab initio QM/MM methods
 
dc.typeArticle
 
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Author Affiliations
  1. The University of Hong Kong
  2. Duke University