journal article·2024-04Open access

Application of the immobilized low-activity waste glass corrosion model to the static dissolution of 24 statistically-designed alkali-borosilicate waste glasses

Sebastien N. Kerisit, James J. Neeway, Charmayne E. Lonergan, Benjamin Parruzot, Jarrod V. Crum, Richard C. Daniel, Gary L. Smith, R. Matthew Asmussen

Abstract

Glass corrosion models that capture the complex mechanisms of the glass-water reaction enable the prediction of nuclear waste glass durability in disposal scenarios. Parameterization of such models is challenging because of the need to capture changes in corrosion behavior with time, reaction conditions, and glass composition. Here, we describe and employ the ILAW (immobilized low-activity waste) glass corrosion model (IGCM) in geochemical simulations of static dissolution tests, at two temperatures (40 °C and 90 °C), for a matrix of 24 enhanced low-activity waste (eLAW) glasses statistically designed to cover a processable composition space defined by 8 major glass components (Al 2O 3, B 2O 3, CaO, Na 2O, SiO 2, SnO 2, ZrO 2, and Others as defined in the text). The IGCM includes a first-order chemical affinity term and an ion-exchange term that represents the net exchange of Na + ions in the pristine glass with protons in aqueous solution. Constant, time-dependent, and time- and pH-dependent functional forms of the ion-exchange term are evaluated to reproduce the change in corrosion behavior with time in saturated, static dissolution tests. The agreement with measured aqueous concentrations of the main glass components (B, Na, and Si) improved significantly upon addition of a time-dependent term, which therefore constitutes a simple representation of the glass-water reaction progress. Due to the limited changes in pH in the static dissolution tests, past a short initial period of rapid increase, addition of a pH-dependent term did not appreciably improve the fits, indicating that comprehensive model parameterization requires more than one type of glass corrosion test to capture a wide range of solution chemistries. IGCM parameters were found to be dependent on glass composition, and the parameter sets generated in this work will enable the development of composition–parameter correlation models that offer the promise of predicting IGCM parameters, and thus glass corrosion behavior, solely based on glass composition.
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Research context

OpenAlex topics: Glass properties and applications · Building materials and conservation · Nuclear materials and radiation effects

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

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