title: Insight on Tricalcium Silicate Hydration and Dissolution Mechanism from Molecular Simulations.
abstract: Hydration of mineral surfaces, a critical process for many technological applications, encompasses multiple coupled chemical reactions and topological changes, challenging both experimental characterization and computational modeling. In this work, we used reactive force field simulations to understand the surface properties, hydration, and dissolution of a model mineral, tricalcium silicate. We show that the computed static quantities, i.e., surface energies and water adsorption energies, do not provide useful insight into predict mineral hydration because they do not account for major structural changes at the interface when dynamic effects are included. Upon hydration, hydrogen atoms from dissociated water molecules penetrate into the crystal, forming a disordered calcium silicate hydrate layer that is similar for most of the surfaces despite wide-ranging static properties. Furthermore, the dynamic picture of hydration reveals the hidden role of surface topology, which can lead to unexpected water tessellation that stabilizes the surface against dissolution.
authors.affiliation: †Molecular Spectroscopy Laboratory, Physical Chemistry Department, University of the Basque Country, Barrio Sarriena s/n, Leioa, 48940 Bizkaia, Spain.
authors.forename: Hegoi
authors.initials: H
authors.lastname: Manzano
authors.affiliation: ‡UNAM-National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology, Bilkent University, Ankara 06800, Turkey.
authors.forename: Engin
authors.initials: E
authors.lastname: Durgun
authors.affiliation: †Molecular Spectroscopy Laboratory, Physical Chemistry Department, University of the Basque Country, Barrio Sarriena s/n, Leioa, 48940 Bizkaia, Spain.
authors.forename: Iñigo
authors.initials: I
authors.lastname: López-Arbeloa
authors.affiliation: §Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
authors.forename: Jeffrey C
authors.initials: JC
authors.lastname: Grossman
keywords: calcium silicate; dissolution; hydration; molecular dynamics; surface properties; water adsorption