期刊
JOURNAL OF CHEMICAL PHYSICS
卷 146, 期 8, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4976686
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资金
- CONACyT
- PAPIIT-UNAM [IN109915]
- CONACYT Basic Science Project [253679]
In this work, a theoretical investigation was made to assess the coordination properties of Pb(II) in [ Pb(H2O)(n)](2+) clusters, with n = 4, 6, 8, 12, and 29, as well as to study proton transfer events, by means of Born-Oppenheimer molecular dynamics simulations at the B3LYP/aug-cc-pVDZ-pp/6-311G level of theory, that were calibrated in comparison with B3LYP/aug-cc-pVDZ-PP/aug-cc-pVDZ calculations. Hemidirected configurations were found in all cases; the radial distribution functions (RDFs) produced well defined first hydration shells (FHSs) for n = 4, 6, 8, and 12, that resulted in a coordination number CN = 4, whereas a clear-cut FHS was not found for n = 29 because the RDF did not have a vacant region after the first maximum; however, three water molecules remained directly interacting with the Pb ion for the whole simulation, while six others stayed at average distances shorter than 4 angstrom but dynamically getting closer and farther, thus producing a CN ranging from 6 to 9, depending on the criterion used to define the first hydration shell. In agreement with experimental data and previous calculations, proton transfer events were observed for n <= 8 but not for n >= 12. For an event to occur, a water molecule in the second hydration shell had to make a single hydrogen bond with a water molecule in the first hydration shell. Published by AIP Publishing.
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