Hydrated proton and hydroxide charge transfer at the liquid/vapor interface of water,The Journal of Chemical Physics

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Hydrated proton and hydroxide charge transfer at the liquid/vapor interface of water
The Journal of Chemical Physics ( IF 3.1 ) Pub Date : 2015-07-23 13:28:40 , DOI: 10.1063/1.4926831
Marielle Soniat ₁ , Revati Kumar ₂ , Steven W. Rick ₁

Affiliation

The role of the solvated excess proton and hydroxide ions in interfacial properties is an interesting scientific question with applications in a variety of aqueous behaviors. The role that charge transfer (CT) plays in interfacial behavior is also an unsettled question. Quantum calculations are carried out on clusters of water with an excess proton or a missing proton (hydroxide) to determine their CT. The quantum results are applied to analysis of multi-state empirical valence bond trajectories. The polyatomic nature of the solvated excess proton and hydroxide ion results in directionally dependent CT, depending on whether a water molecule is a hydrogen bond donor or acceptor in relation to the ion. With polyatomic molecules, CT also depends on the intramolecular bond distances in addition to intermolecular distances. The hydrated proton and hydroxide affect water’s liquid/vapor interface in a manner similar to monatomic ions, in that they induce a hydrogen-bonding imbalance at the surface, which results in charged surface waters. This hydrogen bond imbalance, and thus the charged waters at the surface, persists until the ion is at least 10 Å away from the interface.

中文翻译：

水质/水界面的水合质子和氢氧化物电荷转移

溶剂化的过量质子和氢氧根离子在界面性质中的作用是一个有趣的科学问题，在各种水性行为中都有应用。电荷转移（CT）在界面行为中的作用也是一个悬而未决的问题。对具有过量质子或缺少质子（氢氧化物）的水簇进行量子计算，以确定其CT值。量子结果被应用于多态经验价键轨迹的分析。溶剂化的过量质子和氢氧根离子的多原子性质导致方向依赖的CT，这取决于水分子相对于离子是氢键供体还是受体。对于多原子分子，CT除了分子间距离外，还取决于分子内键的距离。水合的质子和氢氧化物以类似于单原子离子的方式影响水的液/气界面，因为它们在表面上引起氢键不平衡，从而导致带电的地表水。这种氢键不平衡以及表面的带电水一直持续到离子离界面至少10Å为止。

更新日期：2015-07-24

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