Increased Acid Dissociation at the Quartz/Water Interface.
Increased Acid Dissociation at the Quartz/Water Interface.
复制标题
石英/水界面处的酸解离增加。
DOI：
10.1021/acs.jpclett.8b00686
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
M. Sulpizi
中科院分区：
文献类型：
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作者：
Shivam Parashar;Dominika Lesnicki;M. Sulpizi
如相当大量的文献所示，在水表面的酸倾向于是“较少的”酸，这意味着它们的缔合形式优于共轭碱。固液界面发生了什么？在二氧化硅/水界面的情况下，我们展示了吸附分子的酸度如何反而增加。使用自由能微扰方法结合基于电子结构的分子动力学模拟，我们展示了如何在石英/水界面的酸的酸度增加了近两个单位。这种增加的酸度是在界面处的特定微溶剂化的结果，特别是通过石英表面上的硅烷醇和特殊的界面水层稳定去质子化形式的结果。
As shown by a quite significant amount of literature, acids at the water surface tend to be "less" acid, meaning that their associated form is favored over the conjugated base. What happens at the solid/liquid interface? In the case of the silica/water interface, we show how the acidity of adsorbed molecules can instead increase. Using a free energy perturbation approach in combination with electronic structure-based molecular dynamics simulations, we show how the acidity of pyruvic acid at the quartz/water interface is increased by almost two units. Such increased acidity is the result of the specific microsolvation at the interface and, in particular, of the stabilization of the deprotonated form by the silanols on the quartz surface and the special interfacial water layer.