Topological Control of Water Reactivity on Glass Surfaces: Evidence of a Chemically Stable Intermediate Phase

• Published in: The journal of physical chemistry letters 2019-07, Vol.10 (14), p.3955-3960
• Main Authors: Wilkinson, Collin J, Doss, Karan, Hahn, Seung Ho, Keilbart, Nathan, Potter, Arron R, Smith, Nicholas J, Dabo, Ismaila, van Duin, Adri C. T, Kim, Seong H, Mauro, John C
• Format: Article
• Language: English
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/acs.jpclett.9b01275

Glass surfaces are of considerable interest due to their disproportionately large influence on the performance of glass articles in many applications. However, the behavior of glass surfaces has proven difficult to model and predict due to their complex structure and interactions with the environment. Here, the effects of glass network topology on the surface reactivity of glasses have been investigated using reactive and nonreactive force field-based molecular dynamics simulations as well as density functional theory. A topological constraint-based description for surface reactivity is developed, allowing for improved understanding of the physical and chemical origins of surface reactivity. Results show evidence for the existence of a chemically stable intermediate phase on the surface of the glass where the glass network is mechanically isostatic.