Solvation Structure and Ion-Solvent Hydrogen Bonding of Hydrated Fluoride, Chloride and Bromide-A Comparative QM/MM MD Simulation Study

被引:3
作者
Hofer, Thomas S. [1 ]
机构
[1] Univ Innsbruck, Inst Gen Inorgan & Theoret Chem, Ctr Chem & Biomed, Innrain 80-82, A-6020 Innsbruck, Austria
来源
LIQUIDS | 2022年 / 2卷 / 04期
关键词
anionic hydration; hydrogen bonding; aqueous solution; ab initio; molecular dynamics; QM/MM; MOLECULAR-DYNAMICS SIMULATIONS; DENSITY-FUNCTIONAL THEORY; SOLUTIONS DIFFRACTION EXPERIMENTS; ELECTRONIC POPULATION ANALYSIS; GAUSSIAN-TYPE BASIS; MONTE-CARLO; BASIS-SETS; DIELECTRIC-PROPERTIES; COMPUTER-SIMULATIONS; ORBITAL METHODS;
D O I
10.3390/liquids2040026
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
In this study, the correlated resolution-of-identity M & oslash;ller-Plesset perturbation theory of second order (RIMP2) ab initio level of theory has been combined with the newly parameterised, flexible SPC-mTR2 water model to formulate an advanced QM/MM MD simulation protocol to study the solvation properties of the solutes F-, Cl- and Br- in aqueous solution. After the identification of suitable ion-water Lennard-Jones parameters for the QM/MM coupling, a total simulation period of 10 ps (equilibration) plus 25 ps (sampling) could be achieved for each target system at QM/MM conditions. The resulting simulation data enable an in-depth analysis of the respective hydration structure, the first shell ligand exchange characteristics and the impact of solute-solvent hydrogen bonding on the structural properties of first shell water molecules. While a rather unexpected tailing of the first shell ion-oxygen peak renders the identification of a suitable QM boundary region challenging, the presented simulation results provide a valuable primer for more advanced simulation approaches focused on the determination of single-ion thermodynamical properties.
引用
收藏
页码:445 / 464
页数:20
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