Seeded Stage III glass dissolution behavior of a statistically designed glass matrix

Abstract

AbstractThe dissolution rate of some glasses accelerates after prolonged time spent at a slow, residual dissolution rate. This phenomenon is referred to as Stage III behavior. The acceleration in glass dissolution rate linked to Stage III behavior is significant and may be the most impactful behavior to long‐term performance of glass in a repository. This work is aimed at understanding the effect of glass composition on Stage III behavior to add a level of technical defensibility to glass disposal. To this end, a set of 24 glass compositions were statistically designed, where eight glass components (SiO2, B2O3, Al2O3, CaO, Na2O, SnO2, ZrO2, and Others) have been independently varied in order to study the individual effects of each glass component. These glasses have been subjected to static dissolution tests at 90°C in deionized water and then seeded with zeolite Na‐P2 28 days into the testing to induce Stage III behavior. The response of the glasses to the zeolite seeds fell into four primary types: (1) no response to seeds; (2) an immediate linear sustained acceleration in the rate; (3) an immediate linear acceleration in the rate followed by a decrease; and (4) a progressive acceleration in the rate that is concurrent with the addition of the seeds. The main glass components observed to influence these behaviors were CaO, Al2O3, B2O3, and ZrO2, where (1) CaO influenced which glasses showed a Stage III response to seeds (high CaO: types 2, 3, and 4) or did not respond to seeds (low CaO: type 1), (2) Al2O3 and B2O3 influenced which glasses showed a sustainable Stage III response (high Al2O3: types 2 and 4) versus transitory response (low Al2O3 and high B2O3: type 3), and (3) ZrO2 concentration influenced whether glasses showed a linear (high ZrO2: type 2) versus progressive (low ZrO2: type 4) response to seeds.