Department of Chemical Engineering, National Taiwan University of Science and Technology, 43 Keelung Road, Section 4, Taipei 106-07, Taiwan.
J Chem Phys. 2013 Jun 28;138(24):244501. doi: 10.1063/1.4809995.
Water and the organic solvents tetrahydrofuran, 1,3-dioxolane, 1,4-dioxane, 1-propanol, 2-propanol, tert-butanol, acetonitrile, or acetone are completely miscible in all proportions at room temperature. Here, we present new buffering-out phase separation systems that the above mentioned organic aqueous solutions can be induced to form two liquid phases in the presence of a biological buffer 2-[[1,3-dihydroxy-2-(hydroxymethyl)propan-2-yl]amino]ethanesulfonic acid (TES). The lower liquid phase is rich in water and buffer, and the upper phase is organic rich. This observation has both practical and mechanistic interests. The phase diagrams of these systems were constructed by experimental measurements at ambient conditions. Molecular dynamic (MD) simulations were performed for TES + water + THF system to understand the interactions between TES, water, and organic solvent at molecular level. Several composition-sets for this system, beyond and inside the liquid-liquid phase-splitting region, have been simulated. Interestingly, the MD simulation for compositions inside the phase separation region showed that THF molecules are forced out from the water network to start forming a new liquid phase. The hydrogen-bonds, hydrogen-bonds lifetimes, hydrogen-bond energies, radial distribution functions, coordination numbers, the electrostatic interactions, and the van der Waals interactions between the different pairs have been calculated. Additionally, MD simulations for TES + water + tert-butanol∕acetonitrile∕acetone phase separation systems were simulated. The results from MD simulations provide an explanation for the buffering-out phenomena observed in [TES + water + organic solvent] systems by a mechanism controlled by the competitive interactions of the buffer and the organic solvent with water. The molecular mechanism reported here is helpful for designing new benign separation materials.
在室温下,水和有机溶剂四氢呋喃、1,3-二氧杂环戊烷、1,4-二氧六环、1-丙醇、2-丙醇、叔丁醇、乙腈或丙酮完全可以任意比例互溶。在这里,我们提出了新的缓冲分相体系,在生物缓冲液 2-[[1,3-二羟基-2-(羟甲基)丙烷-2-基]氨基]乙磺酸(TES)的存在下,上述有机溶剂水溶液可以诱导形成两相。下相富含水和缓冲液,上相富含有机溶剂。这一观察结果具有实际和机制上的双重意义。通过在环境条件下的实验测量构建了这些体系的相图。对 TES+水+THF 体系进行了分子动力学(MD)模拟,以在分子水平上理解 TES、水和有机溶剂之间的相互作用。对该体系的几个组成集进行了模拟,包括超出和在液-液相分相区域内的组成。有趣的是,在分相区域内的组成的 MD 模拟表明,THF 分子被迫离开水分子网络,开始形成新的液相。计算了不同对之间的氢键、氢键寿命、氢键能、径向分布函数、配位数、静电相互作用和范德华相互作用。此外,还对 TES+水+叔丁醇/乙腈/丙酮分相体系进行了 MD 模拟。MD 模拟的结果为在[TES+水+有机溶剂]体系中观察到的缓冲分相现象提供了一种解释,这种机制受缓冲剂和有机溶剂与水的竞争相互作用控制。这里报道的分子机制有助于设计新的良性分离材料。