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 |
|