Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 123, Issue 43, Pages 9155-9166Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.9b04541
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Funding
- CONACyT
- PAPIIT-UNAIVI [IN110419]
- Miztli-DGTIC-UNAM [LANCAD-UNAM-DGTIC-028]
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The Pb2+ presents unique hydration features that make the experimental characterization and its theoretical modeling challenging: classical molecular dynamics (MD) with standard force-fields fails to produce the experimentally determined diffusion coefficient and the EXAFS spectrum. Here we study the hydration of Pb2+ in aqueous solution employing a polarizable model compatible with the MCDHO water model. The MCDHO FF for the Pb2+-water interaction was fitted to reproduce the configurations and interaction energies of various [Pb(H2O)(n)](2+) clusters obtained with ab initio calculations, with n = 4, 6, and 8. Its use in classical MD simulations yielded qualitative agreement with Born- Oppenheimer molecular dynamics of gas-phase hydrated clusters and MD simulations of the aqueous solution resulted in good agreement with the experimental D-pb(2+) and EXAFS spectrum. Analysis of the MD trajectories revealed a labile and very dynamic hemidirected first hydration shell in the aqueous solution with a non-well-defined coordination number CN; nonetheless, it was found that the more probable hydration structures have either 3 or 4 water molecules directly bound to the Pb2+ with another 3 or 2 at slightly larger distances. The simulations of the gas-phase [Pb(H2O)(29)](2+) cluster were found to capture the main structural features of the diluted aqueous solution.
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