Microsolvation of hydrogen sulfide: exploration of H2S.(H2O)n and SH-.H3O+.(H2O)n-1 (n = 5-7) cluster structures on ab initio potential energy surfaces by the scaled hypersphere search method.
Microsolvation of hydrogen sulfide: exploration of H2S.(H2O)n and SH-.H3O+.(H2O)n-1 (n = 5-7) cluster structures on ab initio potential energy surfaces by the scaled hypersphere search method.
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DOI：
10.1021/jp710494n
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发表时间：
2008-02
期刊：
影响因子：
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通讯作者：
S. Maeda;K. Ohno
中科院分区：
文献类型：
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作者：
S. Maeda;K. Ohno
采用尺度超球搜索方法对H2S.(H2O)n/SH-. h30o +的势能面进行了从头计算。（H2O）n-1体系，n = 5-7。在MP2/6-311++G(3df,2p)//B3LYP/6-31+G**水平上计算，得到n = 5-7的局部最小数据库分别为121、326和553个结构。在这些小簇大小中，SH-. h30 +。（H2O）n-1型相对于H2S仍不稳定。（H2O）n型，以及H2S的全局最小值。（H2O）n与（H2O）n+1的纯水团簇非常相似。基于现有数据库的热力学模拟表明，在低温下，结构从混合良好的（H2O）n+1类整体最小值转变为高温下H2S和（H2O）n之间未混合的配合物。
The scaled hypersphere search method was applied to ab initio potential energy surfaces of the H2S.(H2O)n/SH-.H3O+.(H2O)n-1 system with n = 5-7. Local minima databases including 121, 326, and 553 structures for n = 5-7, respectively, were obtained based on calculations at the MP2/6-311++G(3df,2p)//B3LYP/6-31+G** level. In these small cluster sizes, the SH-.H3O+.(H2O)n-1 type is still unstable relative to the H2S.(H2O)n type, and the global minima for H2S.(H2O)n are very similar to those of pure water clusters of (H2O)n+1. Thermodynamic simulations based on the present databases showed a structure transition from the well-mixed (H2O)n+1-like global minimum at low temperatures to unmixed complexes between H2S and (H2O)n at high temperatures.