Surface structure and stability of partially hydroxylated silica surfaces

Rimsza, J. M.; Jones, R. E.; Criscenti, L. J.

doi:10.1021/acs.langmuir.7b00041

Surface structure and stability of partially hydroxylated silica surfaces

Journal Article · Tue Apr 04 00:00:00 EDT 2017 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.7b00041· OSTI ID:1356827

^[1]; Jones, R. E. ^[2]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Surface energies of silicates influence crack propagation during brittle fracture and decrease with surface relaxation caused by annealing and hydroxylation. Molecular-level simulations are particularly suited for the investigation of surface processes. In this work, classical MD simulations of silica surfaces are performed with two force fields (ClayFF and ReaxFF) to investigate the effect of force field reactivity on surface structure and energy as a function of surface hydroxylation. An unhydroxylated fracture surface energy of 5.1 J/m² is calculated with the ClayFF force field, and 2.0 J/m² is calculated for the ReaxFF force field. The ClayFF surface energies are consistent with the experimental results from double cantilever beam fracture tests (4.5 J/m²), whereas ReaxFF underestimated these surface energies. Surface relaxation via annealing and hydroxylation was performed by creating a low-energy equilibrium surface. Annealing condensed neighboring siloxane bonds increased the surface connectivity, and decreased the surface energies by 0.2 J/m² for ClayFF and 0.8 J/m² for ReaxFF. Posthydroxylation surface energies decreased further to 4.6 J/m² with the ClayFF force field and to 0.2 J/m² with the ReaxFF force field. Experimental equilibrium surface energies are ~0.35 J/m², consistent with the ReaxFF force field. Although neither force field was capable of replicating both the fracture and equilibrium surface energies reported from experiment, each was consistent with one of these conditions. Furthermore, future computational investigations that rely on accurate surface energy values should consider the surface state of the system and select the appropriate force field.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Sandia National Laboratories, Livermore, CA

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1356827

Report Number(s):: SAND2017-2690J; 651669

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 15 Vol. 33; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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