Hygroscopic Growth of Adsorbed Water Films on Smectite Clay Particles
Abstract
Hygroscopic growth of adsorbed water films on clay particles underlies a number of environmental science questions, from the air quality and climate impacts of mineral dust aerosols to the hydrology and mechanics of unsaturated soils and sedimentary rocks. Here, we use molecular dynamics (MD) simulations to establish the relation between adsorbed water film thickness (h) and relative humidity (RH) or disjoining pressure (Π), which has long been uncertain due to factors including sensitivity to particle shape, surface roughness, and aqueous chemistry. We present a new MD simulation approach that enables precise quantification of Π in films up to six water monolayers thick. We find that the hygroscopicity of phyllosilicate mineral surfaces increases in the order mica < K-smectite < Na-smectite. The relationship between Π and h on clay surfaces follows a double exponential decay with e-folding lengths of 2.3 and 7.5 Å. The two decay length scales are attributed to hydration repulsion and osmotic phenomena in the electrical double layer (EDL) at the clay–water interface.
- Authors:
-
- Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, United States
- Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, United States, High Meadows Environmental Institute, Princeton University, Princeton, New Jersey 08544, United States
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 2274869
- Alternate Identifier(s):
- OSTI ID: 2281644
- Grant/Contract Number:
- SC0018419; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Name: Environmental Science and Technology Journal Volume: 58 Journal Issue: 2; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; MD simulations; clay minerals; water films; disjoining pressure; hygroscopic growth; dust aerosols; unsaturated soils
Citation Formats
Li, Xiaohan, and Bourg, Ian C. Hygroscopic Growth of Adsorbed Water Films on Smectite Clay Particles. United States: N. p., 2024.
Web. doi:10.1021/acs.est.3c08253.
Li, Xiaohan, & Bourg, Ian C. Hygroscopic Growth of Adsorbed Water Films on Smectite Clay Particles. United States. https://doi.org/10.1021/acs.est.3c08253
Li, Xiaohan, and Bourg, Ian C. Tue .
"Hygroscopic Growth of Adsorbed Water Films on Smectite Clay Particles". United States. https://doi.org/10.1021/acs.est.3c08253.
@article{osti_2274869,
title = {Hygroscopic Growth of Adsorbed Water Films on Smectite Clay Particles},
author = {Li, Xiaohan and Bourg, Ian C.},
abstractNote = {Hygroscopic growth of adsorbed water films on clay particles underlies a number of environmental science questions, from the air quality and climate impacts of mineral dust aerosols to the hydrology and mechanics of unsaturated soils and sedimentary rocks. Here, we use molecular dynamics (MD) simulations to establish the relation between adsorbed water film thickness (h) and relative humidity (RH) or disjoining pressure (Π), which has long been uncertain due to factors including sensitivity to particle shape, surface roughness, and aqueous chemistry. We present a new MD simulation approach that enables precise quantification of Π in films up to six water monolayers thick. We find that the hygroscopicity of phyllosilicate mineral surfaces increases in the order mica < K-smectite < Na-smectite. The relationship between Π and h on clay surfaces follows a double exponential decay with e-folding lengths of 2.3 and 7.5 Å. The two decay length scales are attributed to hydration repulsion and osmotic phenomena in the electrical double layer (EDL) at the clay–water interface.},
doi = {10.1021/acs.est.3c08253},
journal = {Environmental Science and Technology},
number = 2,
volume = 58,
place = {United States},
year = {Tue Jan 02 00:00:00 EST 2024},
month = {Tue Jan 02 00:00:00 EST 2024}
}
https://doi.org/10.1021/acs.est.3c08253
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