Journal
JOURNAL OF THE MECHANICS AND PHYSICS OF SOLIDS
Volume 60, Issue 9, Pages 1660-1675Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.jmps.2012.04.015
Keywords
Water sorption; Hysteresis; Condensation; Porous media; Nanopore; Concrete
Funding
- NSF [1153509, 1153494, DMS-0948071, CMS-0556323]
- U.S. DoT through the Infrastructure Technology Institute of Northwestern University [27323]
- Direct For Mathematical & Physical Scien [0854905] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1153509] Funding Source: National Science Foundation
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1153494, 1129449] Funding Source: National Science Foundation
- Division Of Mathematical Sciences [0854905] Funding Source: National Science Foundation
- Division Of Mathematical Sciences
- Direct For Mathematical & Physical Scien [0948071] Funding Source: National Science Foundation
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Motivated by the puzzle of sorption hysteresis in Portland cement concrete or cement paste, we develop in Part II of this study a general theory of vapor sorption and desorption from nanoporous solids, which attributes hysteresis to hindered molecular condensation with attractive lateral interactions. The classical mean-field theory of van der Waals is applied to predict the dependence of hysteresis on temperature and pore size, using the regular solution model and gradient energy of Cahn and Hilliard. A simple hierarchical wetting model for thin nanopores is developed to describe the case of strong wetting by the first monolayer, followed by condensation of nanodroplets and nanobubbles in the bulk. The model predicts a larger hysteresis critical temperature and enhanced hysteresis for molecular condensation across nanopores at high vapor pressure than within monolayers at low vapor pressure. For heterogeneous pores, the theory predicts sorption/desorption sequences similar to those seen in molecular dynamics simulations, where the interfacial energy (or gradient penalty) at nanopore junctions acts as a free energy barrier for snap-through instabilities. The model helps to quantitatively understand recent experimental data for concrete or cement paste wetting and drying cycles and suggests new experiments at different temperatures and humidity sweep rates. (C) 2012 Elsevier Ltd. All rights reserved.
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