带电界面处界面水的反离子效应及其与霍夫迈斯特级数的相关性,Journal of the American Chemical Society

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带电界面处界面水的反离子效应及其与霍夫迈斯特级数的相关性
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2014-04-17 , DOI: 10.1021/ja412952y
Satoshi Nihonyanagi _{1,

2} , Shoichi Yamaguchi _{1,

2} , Tahei Tahara _{1,

2}

Affiliation

以霍夫迈斯特级数为代表的特定反离子效应对于蛋白质沉淀、电解质溶液的表面张力、表面活性剂的相变等多种现象都很重要。带电界面处的界面水，并讨论了与 Hofmeister 系列相关的观察到的效应。对带正电荷的十六烷基三甲基铵单层/电解质溶液界面和带负电荷的十二烷基硫酸盐单层/电解质界面的模型系统进行了实验。在带正电的界面处，界面水的 OH 带强度以霍夫迈斯特级数的顺序减小，表明卤化物阴离子在界面上的吸附性决定了之前由 Zhang 和 Cremer 提出的 Hofmeister 顺序（Curr. Opin. Chem. Biol. 2006, 10, 658-663）。另一方面，在带负电荷的界面上，OH 带强度不显着依赖于抗衡阳离子，而界面水的氢键强度的变化与阳离子效应的霍夫迈斯特级密切相关。这些结果为阴离子和阳离子霍夫迈斯特效应的分子水平机制提供了新的见解。而界面水的氢键强度的变化与阳离子效应的霍夫迈斯特级密切相关。这些结果为阴离子和阳离子霍夫迈斯特效应的分子水平机制提供了新的见解。而界面水的氢键强度的变化与阳离子效应的霍夫迈斯特级密切相关。这些结果为阴离子和阳离子霍夫迈斯特效应的分子水平机制提供了新的见解。

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Counterion Effect on Interfacial Water at Charged Interfaces and Its Relevance to the Hofmeister Series

Specific counterion effects represented by Hofmeister series are important for a variety of phenomena such as protein precipitations, surface tensions of electrolytes solutions, phase transitions of surfactants, etc. We applied heterodyne-detected vibrational sum-frequency generation spectroscopy to study the counterion effect on the interfacial water at charged interfaces and discussed the observed effect with relevance to the Hofmeister series. Experiments were carried out for model systems of positively charged cetyltrimethylammonium monolayer/electrolyte solution interface and negatively charged dodecylsulfate monolayer/electrolyte interface. At the positively charged interface, the intensity of the OH band of the interfacial water decreases in the order of the Hofmeister series, suggesting that the adsorbability of halide anions onto the interface determines the Hofmeister order as previously proposed by Zhang and Cremer (Curr. Opin. Chem. Biol. 2006, 10, 658-663). At the negatively charged interfaces, on the other hand, the OH band intensity does not depend significantly on the countercation, whereas variation in the hydrogen-bond strength of the interfacial water is well correlated with the Hofmeister order of the cation effect. These results provide new insights into the molecular level mechanisms of anionic and cationic Hofmeister effects.

更新日期：2014-04-17

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