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Entropy-Enthalpy Compensation in Peptide Adsorption on Solid Surfaces: Dependence on Surface Hydration.
Langmuir ( IF 3.9 ) Pub Date : 2020-08-19 , DOI: 10.1021/acs.langmuir.0c01845
Xiang Wang 1 , Xiao Yang 1 , Huijun Chen 2 , Xiaoning Yang 1 , Zhijun Xu 1, 3
Affiliation  

Although protein adsorption at the solid–water interface is of immense importance, understanding the crucial role of the water phase in mediating protein–surface interactions is lacking, particularly due to the lack of fundamental thermodynamic data. Herein, we have performed complicated free energy calculations and successfully extracted the entropy and enthalpy changes of molecular adsorption on solids. Using the gold and graphene as the surface models with distinct affinities to the water phase, we successfully unravel the sharply opposite manners of entropy–enthalpy compensation in driving water and tripeptide adsorptions on two surfaces. Though the thermodynamic features of water adsorption on surface are enthalpically dominated based on the positions of free energy barriers and minima, the favorable entropy term significantly decreases the free energy barrier and further stabilizes the adsorbate at the adsorption site on the graphene surface. For the peptide, the shape of the adsorption free energy profile is jointly determined by the enthalpy and entropy changes, which, however, alternatively act the driving force to promote the peptide adsorption on the Au surface and graphene surface. The distinct structural and dynamic properties of solid–liquid interfaces account for the special role of the interfacial water phase in regulating the competitive relationship between the entropy and enthalpy variations.

中文翻译:

固体表面上肽吸附的熵焓补偿:取决于表面水化作用。

尽管蛋白质在固-水界面的吸附极为重要,但由于缺乏基本的热力学数据,因此缺乏对水相在介导蛋白质-表面相互作用中的关键作用的了解。在这里,我们进行了复杂的自由能计算,并成功地提取了分子吸附在固体上的熵和焓变化。使用金和石墨烯作为与水相具有独特亲和力的表面模型,我们成功地揭示了驱动水和三肽在两个表面上吸附的熵-焓补偿的截然相反的方式。尽管基于自由能垒和极小值的位置,水吸附在表面上的热力学特征在焓上占主导地位,有利的熵项显着降低了自由能垒,并进一步稳定了石墨烯表面吸附位点的被吸附物。对于肽,吸附自由能曲线的形状由焓和熵的变化共同确定,但是,它们交替地作用驱动力以促进肽在Au表面和石墨烯表面上的吸附。固液界面的独特结构和动力学特性说明了界面水相在调节熵变和焓变之间的竞争关系中的特殊作用。然而,其可替代地充当驱动力以促进肽在Au表面和石墨烯表面上的吸附。固液界面的独特结构和动力学特性说明了界面水相在调节熵变和焓变之间的竞争关系中的特殊作用。然而,其可替代地充当驱动力以促进肽在Au表面和石墨烯表面上的吸附。固液界面的独特结构和动力学特性说明了界面水相在调节熵变和焓变之间的竞争关系中的特殊作用。
更新日期:2020-09-15
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