Curvature-induced hydrophobicity at imogolite–water interfaces

Fernandez-Martinez, Alejandro; Tao, Jinhui; Wallace, Adam F.; Bourg, Ian C.; Johnson, Mark R.; De Yoreo, James J.; Sposito, Garrison; Cuello, Gabriel J.; Charlet, Laurent

doi:10.1039/d0en00304b

Title: Curvature-induced hydrophobicity at imogolite–water interfaces

Journal Article · Fri Aug 14 00:00:00 EDT 2020 · Environmental Science: Nano

DOI:https://doi.org/10.1039/d0en00304b· OSTI ID:1677642

^[1];

^[2]; Wallace, Adam F. ^[3];

^[4]; Johnson, Mark R. ^[5]; De Yoreo, James J. ^[6]; Sposito, Garrison ^[7]; Cuello, Gabriel J. ^[5];

^[1]

Univ. Grenoble Alpes (France); Univ. Savoie Mont Blanc (France)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Delaware, Newark, DE (United States)
Princeton Univ., NJ (United States)
Inst. Laue-Langevin (ILL), Grenoble (France)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Univ. of California, Berkeley, CA (United States)

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. In this work, 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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC) and The Molecular Foundry (TMF); Princeton Univ., NJ (United States)

Sponsoring Organization:: Région Rhône-Alpes; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-76RL01830; SC0018439; SC0018419; AC02-05CH11231; KC020105-FWP12152

OSTI ID:: 1677642

Alternate ID(s):: OSTI ID: 1647501; OSTI ID: 1784310

Report Number(s):: PNNL-SA-155958

Journal Information:: Environmental Science: Nano, Vol. 7, Issue 9; ISSN 2051-8153

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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