Mechanistic Understanding of Glass-Water Reaction
EMSL Project ID
40084
Abstract
The construction of valid rate models, such as the Transition State Theory Kinetic Rate Equation, to describe the dissolution of rock-forming minerals, the evolution of soils, and the corrosion resistance of engineered materials for numerous applications lies at heart of the predictive science of geochemistry. As a result, there has been and continues to be broad interest in the processes that govern water-mineral and water-glass interactions by the geochemical community. Furthermore, the interest of immobilizing radioactive waste in alkali alumino-borosilicate glasses has resulted in a large number of experimental studies that used laboratory-scale experiments to understand the long-term weathering of nuclear waste glasses [see Pierce et al. and colleagues (2008; 2010; 2008a; 2008b) for additional details]. To develop an improved predictive understanding of the long-term weathering of nuclear waste glasses, requires the ability to mathematically describe key coupled-processes (e.g., physical and chemical) that control the glass-water reaction across a wide variety of spatial- and temporal-scales. Although the importance of key coupled physical and chemical processes change with the different stages of the glass weathering, developing an understanding of the formation of alteration phases (e.g., typically an amorphous hydrated surface layer) and how each stage relates to the initial glass structure is a critical component needed to improve our predictive understanding. An improved understanding of alteration phase formation requires a combination of molecular-scale techniques (namely Nuclear Magnetic Resonance), laboratory-scale dissolution experiments, and atomistic and continuum-scale computational simulations of the glass water reaction.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2010-10-03
End Date
2012-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Bacon DH, and EM Pierce. 2010. Sensitivity Analysis of Kinetic Rate-Law Parameters Used to Simulate Long-Term Weathering of ILAW Glass . PNNL-19472, Pacific Northwest National Laboratory, Richland, WA.
Kerisit SN, and EM Pierce. 2011. "Monte Carlo Simulations of the Dissolution of Borosilicate and Aluminoborosilicate Glasses in Dilute Aqueous Solutions." Geochimica et Cosmochimica Acta 75(18):5296-5309. doi:10.1016/j.gca.2011.06.036
Kerisit SN, and EM Pierce. 2012. "Monte Carlo Simulations of the Dissolution of Borosilicate Glasses in Near-Equilibrium Conditions." Journal of Non-crystalline Solids 358(10):1324-1332. doi:10.1016/j.jnoncrysol.2012.03.003.
Kerisit SN, JV Ryan, and EM Pierce. 2013. "Monte Carlo Simulations of the Corrosion of Aluminoborosilicate Glasses." PNNL-SA-95303, Pacific Northwest National Laboratory, Richland, WA. [Unpublished]
Pierce EM, and DH Bacon. 2011. "Combined Experimental and Computational Approach to Predict the Glass-Water Reaction." Nuclear Technology 176(1):22-39.
Pierce EM, DH Bacon, SN Kerisit, CF Windisch, Jr, KJ Cantrell, MM Valenta, SD Burton, RJ Serne, and SV Mattigod. 2010. Integrated Disposal Facility FY2010 Glass Testing Summary Report . PNNL-19736, Pacific Northwest National Laboratory, Richland, WA.
Windisch CF, Jr, EM Pierce, SD Burton, and CC Bovaird. 2011. "Deep-UV Raman spectroscopic analysis of structure and dissolution rates of silica-rich sodium borosilicate glasses." Journal of Non-crystalline Solids 357(10):2170-2177. doi:10.1016/j.jnoncrysol.2011.02.046