Curvature-induced hydrophobicity at imogolite–water interfaces,Environmental Science: Nano

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Curvature-induced hydrophobicity at imogolite–water interfaces
Environmental Science: Nano ( IF 5.8 ) Pub Date : 2020-08-14 , DOI: 10.1039/d0en00304b
Alejandro Fernandez-Martinez _{1,

2,

3,

4,

5} , Jinhui Tao _{6,

7,

8,

9} , Adam F. Wallace _{9,

10,

11,

12} , Ian C. Bourg _{9,

13,

14,

15,

16} , Mark R. Johnson _{17,

18,

19} , James J. De Yoreo _{6,

7,

8,

9,

20} , Garrison Sposito _{9,

21,

22,

23} , Gabriel J. Cuello _{17,

18,

19} , Laurent Charlet _{1,

2,

3,

4,

5}

Affiliation

Université Grenoble Alpes
Université Savoie Mont Blanc
CNRS
IRD
IFSTTAR
Physical and Computational Sciences Directorate
Pacific Northwest National Laboratory
Richland
USA
Department of Earth Sciences
University of Delaware
Newark
Department of Civil and Environmental Engineering
Princeton Environmental Institute
Princeton University
Princeton
Institut Laue Langevin
38000 Grenoble
France
Department of Materials Science and Engineering
Department of Environmental Science, Policy, and Management
University of California
Berkeley

Imogolite, a nanotubular aluminosilicate mineral, is commonly found in volcanic soils, where it exerts a control on carbon dynamics. Synthetic imogolites are used for the removal of contaminants from industrial effluents and are considered for a range of other applications including gas adsorption and functionalised heterogeneous catalysts. In spite of their environmental and industrial relevance, the properties of imogolite–water interfaces remain poorly understood. Here, an experimental and computational study is presented in which the structure and energetics of water are characterized on the curved external surface of imogolite and the hydrophilicity of this surface is contrasted with that of gibbsite, its planar counterpart. Atomic force spectroscopy experiments show that in spite of their identical surface structure, imogolite has a lower hygroscopicity than gibbsite. Molecular dynamics simulations provide an explanation for this observation: the curvature of imogolite prevents the formation of in-plane H-bonds along the directions of the nanotube circumference, lowering the enthalpy of adsorption of water molecules. The different arrangement of surface H-bonds and the resulting differences in hydration properties also affects the acidity constants of surface hydroxyl groups. This ‘nanotube effect’ may be relevant to other nanotubular systems with high curvatures, potentially impacting their wetting properties, their colloidal stability and their affinity towards hydrophobic organic moieties.

中文翻译：

弯曲在水硬石-水界面处的疏水性

火山岩中常见的纳米管状硅铝酸盐矿物-Imogolite，可控制碳动力学。合成的卵黄石用于去除工业废水中的污染物，并被考虑用于一系列其他应用，包括气体吸附和功能化的多相催化剂。尽管它们与环境和工业相关，但对依云母-水界面的性质仍然知之甚少。在这里，进行了一项实验和计算研究，其中水的结构和能量学特征在依云母的弯曲外表面上进行了表征，并且该表面的亲水性与水铝石的平面亲水性形成对比。原子力光谱实验表明，尽管它们具有相同的表面结构，卵黄石的吸湿性低于三水铝石。分子动力学模拟为这一观察提供了解释：依维戈石的曲率阻止了沿纳米管圆周方向形成平面内H键，从而降低了水分子的吸附焓。表面氢键的不同排列以及由此产生的水合性质差异也影响表面羟基的酸度常数。这种“纳米管效应”可能与其他具有高曲率的纳米管系统有关，可能会影响其润湿性，胶体稳定性以及对疏水性有机基团的亲和力。萤石的曲率阻止了沿着纳米管圆周方向形成平面内H键，从而降低了水分子的吸附焓。表面氢键的不同排列以及水合性质的不同也会影响表面羟基的酸度常数。这种“纳米管效应”可能与其他具有高曲率的纳米管系统有关，可能会影响其润湿性，胶体稳定性以及对疏水性有机基团的亲和力。萤石的曲率阻止了沿着纳米管圆周方向形成平面内H键，从而降低了水分子的吸附焓。表面氢键的不同排列以及水合性质的不同也会影响表面羟基的酸度常数。这种“纳米管效应”可能与其他具有高曲率的纳米管系统有关，可能会影响其润湿性，胶体稳定性以及对疏水性有机基团的亲和力。

更新日期：2020-09-18

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