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Elucidating solvent contributions to solution reactions with ab initio QM/MM methods.

dc.contributor.author Hu, Hao
dc.contributor.author Yang, Weitao
dc.coverage.spatial United States
dc.date.accessioned 2011-06-21T17:26:40Z
dc.date.issued 2010-03-04
dc.identifier http://www.ncbi.nlm.nih.gov/pubmed/20121225
dc.identifier.uri https://hdl.handle.net/10161/4075
dc.description.abstract Computer 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 S(N)2 reaction of CH(3)Cl + 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.
dc.language eng
dc.language.iso en_US
dc.publisher American Chemical Society (ACS)
dc.relation.ispartof J Phys Chem B
dc.relation.isversionof 10.1021/jp905886q
dc.subject Catalysis
dc.subject Computer Simulation
dc.subject Enzymes
dc.subject Protein Conformation
dc.subject Quantum Theory
dc.subject Solutions
dc.subject Solvents
dc.subject Thermodynamics
dc.title Elucidating solvent contributions to solution reactions with ab initio QM/MM methods.
dc.title.alternative
dc.type Journal article
duke.contributor.id Yang, Weitao|0110948
dc.description.version Version of Record
duke.date.pubdate 2010-3-4
duke.description.issue 8
duke.description.volume 114
dc.relation.journal Journal of Physical Chemistry B
pubs.author-url http://www.ncbi.nlm.nih.gov/pubmed/20121225
pubs.begin-page 2755
pubs.end-page 2759
pubs.issue 8
pubs.organisational-group Chemistry
pubs.organisational-group Duke
pubs.organisational-group Physics
pubs.organisational-group Trinity College of Arts & Sciences
pubs.publication-status Published
pubs.volume 114
dc.identifier.eissn 1520-5207


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