Dynamics of Water in the Solvation Shell of an Iodate Ion: A Born-Oppenheimer Molecular Dynamics Study

被引:5
作者
Sharma, Bikramjit [1 ]
Chandra, Amalendu [1 ]
机构
[1] Indian Inst Technol, Dept Chem, Kanpur 208016, Uttar Pradesh, India
关键词
QMCF MD SIMULATION; AQUEOUS-SOLUTION; ELECTRON LOCALIZATION; SPECTRAL DIFFUSION; HYDRATION SHELLS; JUMP MECHANISM; SALT-SOLUTIONS; LIQUID WATER; SULFATE; PHOSPHATE;
D O I
10.1021/acs.jpcb.9b12008
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The iodate ion has an anisotropic structure and charge distribution. It has a pyramidal shape with the iodine atom located at the peak of the pyramid. The water molecules interact differently with the positively charged iodine and the negatively charged oxygen atoms of this anion, giving rise to two distinct solvation shells. In the present study, we have performed ab initio Born-Oppenheimer molecular dynamics simulations to investigate the dynamics of water molecules in the iodine and oxygen solvation shells of the iodate ion and compared the behavior with those of the bulk. The dynamics of water is calculated for both the BLYP and the dispersion-corrected BLYP-D3 functionals at room temperature. The dynamics of water in the solvation shells at higher temperatures of 353 and 330 K has also been investigated for the BLYP and BLYP-D3 functionals, respectively. The hydrogen bond dynamics, vibrational spectral diffusion, orientational and translational diffusion, and residence dynamics of water molecules in the two solvation shells are looked at in the current study. The ion-water hydrogen bond dynamics is found to be somewhat faster than that for water-water hydrogen bonds in the bulk, which can be attributed to a ring-like electron distribution on the iodate oxygens. The dynamical trends are connected to the water structure making/breaking properties of the positively charged iodine and negatively charged oxygen sites of the anion. Furthermore, orientational jumps of the iodate ion and also those of surrounding water molecules which are hydrogen bonded to the oxygen atoms of the iodate ion are also investigated. It is found that the nature of these orientational jumps can be different from those reported earlier for planar polyoxyanions such as the nitrate ion.
引用
收藏
页码:2618 / 2631
页数:14
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