Monte Carlo Simulations of the Dissolution of Borosilicate Glasses in Near-Equilibrium Conditions

Journal Article · Tue May 15 04:00:00 EDT 2012 · Journal of Non-crystalline Solids, 358(10):1324-1332

DOI:https://doi.org/10.1016/j.jnoncrysol.2012.03.003· OSTI ID:1043104

Kerisit, Sebastien N; Pierce, Eric M

Monte Carlo simulations were performed to investigate the mechanisms of glass dissolution as equilibrium conditions are approached in both static and flow-through conditions. The glasses studied are borosilicate glasses in the compositional range (80-x)% SiO2 (10+x/2)% B2O3 (10+x/2)% Na2O, where 5 < x < 30%. In static conditions, dissolution/condensation reactions lead to the formation, for all compositions studied, of a blocking layer composed of polymerized Si sites with principally 4 connections to nearest Si sites. This layer forms atop the altered glass layer and shows similar composition and density for all glass compositions considered. In flow-through conditions, three main dissolution regimes are observed: at high flow rates, the dissolving glass exhibits a thin alteration layer and congruent dissolution; at low flow rates, a blocking layer is formed as in static conditions but the simulations show that water can occasionally break through the blocking layer causing the corrosion process to resume; and, at intermediate flow rates, the glasses dissolve incongruently with an increasingly deepening altered layer. The simulation results suggest that, in geological disposal environments, small perturbations or slow flows could be enough to prevent the formation of a permanent blocking layer.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1043104
• Report Number(s): PNNL-SA-84928; 40084; 830403000
• Journal Information: Journal of Non-crystalline Solids, 358(10):1324-1332, Journal Name: Journal of Non-crystalline Solids, 358(10):1324-1332
• Country of Publication: United States
• Language: English

Related Subjects

Environmental Molecular Sciences Laboratory
Monte Carlo simulations
borosilicate glasses
glass dissolution