Du Hao, Rasaiah Jayendran C, Miller Jan D
Department of Metallurgical Engineering, 135 South 1460 East, 412 William C. Browning Building, University of Utah, Salt Lake City, Utah 84112, USA.
J Phys Chem B. 2007 Jan 11;111(1):209-17. doi: 10.1021/jp064659o.
The physicochemical properties of alkali halide solutions have long been attributed to the collective interactions between ions and water molecules in the solution, yet the structure of water in these systems and its effect on the equilibrium and dynamic properties of these systems are not clearly understood. Here, we present a systematic view of water structure in concentrated alkali halide solutions using molecular dynamics simulations. The results of the simulations show that the size of univalent ions in the solution has a significant effect on the dynamics of ions and other transport properties such as the viscosity that are correlated with the structural properties of water in aqueous ionic solution. Small cations (e.g., Li+) form electrostatically stabilized hydrophilic hydration shells that are different from the hydration shells of large ions (e.g., Cs+) which behave more like neutral hydrophobic particles, encapsulated by hydrogen-bonded hydration cages. The properties of solutions with different types of ion solvation change in different ways as the ion concentration increases. Examples of this are the diffusion coefficients of the ions and the viscosities of solutions. In this paper we use molecular dynamics (MD) simulations to study the changes in the equilibrium and transport properties of LiCl, RbCl, and CsI solutions at concentrations from 0.22 to 3.97 M.
长期以来,碱金属卤化物溶液的物理化学性质一直被归因于溶液中离子与水分子之间的集体相互作用,然而,这些体系中水的结构及其对这些体系平衡和动力学性质的影响尚不清楚。在此,我们利用分子动力学模拟给出了浓碱金属卤化物溶液中水结构的系统观点。模拟结果表明,溶液中单价离子的大小对离子动力学及其他传输性质(如与离子水溶液中水的结构性质相关的粘度)有显著影响。小阳离子(如Li+)形成静电稳定的亲水性水合壳层,这与大离子(如Cs+)的水合壳层不同,大离子的行为更像是被氢键水合笼包裹的中性疏水颗粒。随着离子浓度的增加,具有不同类型离子溶剂化作用的溶液性质以不同方式变化。离子扩散系数和溶液粘度就是这样的例子。在本文中,我们利用分子动力学(MD)模拟研究了浓度为0.22至3.97 M的LiCl、RbCl和CsI溶液的平衡和传输性质的变化。