期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 9, 页码 3047-3060出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201202821
关键词
ab initio calculations; calcium; cations; solvent effects; water chemistry; XAFS
资金
- US Department of Energy (DOE) Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-FG02-10ER1 6126]
- Department of Energy's Office of Biological and Environmental Research
- US DOE [DE-AC02-06CH11357]
- NSERC (Canada)
- US Department of Energy
Herein, we report on the structure and dynamics of the aqueous Ca2+ system studied by using abinitio molecular dynamics (AIMD) simulations. Our detailed study revealed the formation of well-formed hydration shells with characteristics that were significantly different to those of bulk water. To facilitate a robust comparison with state-of-the-art X-ray absorption fine structure (XAFS) data, we employ a 1st principles MD-XAFS procedure and directly compare simulated and experimental XAFS spectra. A comparison of the data for the aqueous Ca2+ system with those of the recently reported Zn2+, Fe3+, and Al3+ species showed that many of their structural characteristics correlated well with charge density on the cation. Some very important exceptions were found, which indicated a strong sensitivity of the solvent structure towards the cations valence electronic structure. Average dipole moments for the 2nd shell of all cations were suppressed relative to bulk water.
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