Curvature-induced hydrophobicity at imogolite–water interfaces
Abstract
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, theirmore »
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- 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 Org.:
- 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)
- OSTI Identifier:
- 1677642
- Alternate Identifier(s):
- OSTI ID: 1647501; OSTI ID: 1784310
- Report Number(s):
- PNNL-SA-155958
Journal ID: ISSN 2051-8153
- Grant/Contract Number:
- AC05-76RL01830; SC0018439; SC0018419; AC02-05CH11231; KC020105-FWP12152
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science: Nano
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 9; Journal ID: ISSN 2051-8153
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 58 GEOSCIENCES; 54 ENVIRONMENTAL SCIENCES; mineral; water; interface; hydrophilicity
Citation Formats
Fernandez-Martinez, Alejandro, Tao, Jinhui, Wallace, Adam F., Bourg, Ian C., Johnson, Mark R., De Yoreo, James J., Sposito, Garrison, Cuello, Gabriel J., and Charlet, Laurent. Curvature-induced hydrophobicity at imogolite–water interfaces. United States: N. p., 2020.
Web. doi:10.1039/d0en00304b.
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. Curvature-induced hydrophobicity at imogolite–water interfaces. United States. https://doi.org/10.1039/d0en00304b
Fernandez-Martinez, Alejandro, Tao, Jinhui, Wallace, Adam F., Bourg, Ian C., Johnson, Mark R., De Yoreo, James J., Sposito, Garrison, Cuello, Gabriel J., and Charlet, Laurent. Fri .
"Curvature-induced hydrophobicity at imogolite–water interfaces". United States. https://doi.org/10.1039/d0en00304b. https://www.osti.gov/servlets/purl/1677642.
@article{osti_1677642,
title = {Curvature-induced hydrophobicity at imogolite–water interfaces},
author = {Fernandez-Martinez, Alejandro and Tao, Jinhui and Wallace, Adam F. and Bourg, Ian C. and Johnson, Mark R. and De Yoreo, James J. and Sposito, Garrison and Cuello, Gabriel J. and Charlet, Laurent},
abstractNote = {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.},
doi = {10.1039/d0en00304b},
journal = {Environmental Science: Nano},
number = 9,
volume = 7,
place = {United States},
year = {Fri Aug 14 00:00:00 EDT 2020},
month = {Fri Aug 14 00:00:00 EDT 2020}
}
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