Stabilization of Hydroxide Ions at the Interface of a Hydrophobic Monolayer on Water via Reduced Proton Transfer
Stabilization of Hydroxide Ions at the Interface of a Hydrophobic Monolayer on Water via Reduced Proton Transfer
复制标题
通过减少质子转移稳定疏水单分子层界面处的氢氧根离子
DOI：
10.1103/physrevlett.125.156803
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发表时间：
2020
影响因子：
8.6
通讯作者：
Tian Chuanshan
中科院分区：
文献类型：
--
作者：
Yang Shanshan;Chen Mohan;Su Yudan;Xu Jianhang;Wu Xifan;Tian Chuanshan
我们报告了一项联合研究，分别使用表面比和频率振动谱和初始分子动力学模拟，对原始疏水（亚）单层己烷-水界面，即具有不同己烷蒸汽压和差异水的己烷/水界面进行了研究。我们提供了明确的证据，表明水中的己烷以一种稳定超配溶剂化结构的方式改变了界面水结构，并减缓了氢氧根离子（）相对于在大量水中的迁移。这一机制有效地将它们吸引到疏水界面上。结果表明，水合物的质子转移在界面处与在本体处存在显著差异，这是造成疏水界面处本征电荷效应的原因。
We report a joint study using surface-specific sum-frequency vibrational spectroscopy andab initiomolecular dynamics simulations, respectively, on a pristine hydrophobic (sub)monolayer hexane-water interface, namely, the hexane/water interface with varied vapor pressures of hexane and differentin water. We show clear evidence that hexane on water revises the interfacial water structure in a way that stabilizes the hypercoordinated solvation structure and slows down the migration of hydroxide ion () relative to that in bulk water. This mechanism effectively attracts theto the water-hydrophobic interface with respect to its counterion. The result illustrates the striking difference of proton transfer of hydratedat the interface and in the bulk, which is responsible for the intrinsic charging effect at the hydrophobic interface.