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

Collin J Wilkinson; Karan Doss; Seung Ho Hahn; Nathan Keilbart; Arron R Potter; Nicholas J Smith; Ismaila Dabo; Adri C T van Duin; Seong H Kim; John C Mauro

doi:10.1021/acs.jpclett.9b01275

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

J Phys Chem Lett. 2019 Jul 18;10(14):3955-3960. doi: 10.1021/acs.jpclett.9b01275. Epub 2019 Jul 2.

Authors

Collin J Wilkinson¹, Karan Doss¹, Seung Ho Hahn², Nathan Keilbart¹, Arron R Potter³, Nicholas J Smith^{4

5}, Ismaila Dabo^{1

5}, Adri C T van Duin^{1

2

5

6}, Seong H Kim^{1

5

6}, John C Mauro^{1

5}

Affiliations

¹ Department of Materials Science and Engineering , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
² Department of Mechanical Engineering , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
³ Department of Materials Science and Engineering , Rensselaer Polytechnic Institute , Troy , New York 12180 , United States.
⁴ Science and Technology Division , Corning Incorporated , Corning , New York 14831 , United States.
⁵ Materials Research Institute , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
⁶ Department of Chemical Engineering , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.

PMID: 31241951
DOI: 10.1021/acs.jpclett.9b01275

Abstract

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.