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Title: The dissolution behavior of borosilicate glasses in far-from equilibrium conditions

Abstract

In far-from-equilibrium conditions, the dissolution of borosilicate glasses used to immobilize nuclear waste is known to be a function of both temperature and pH. The aim of this paper is to study effects of these variables on three model waste glasses (SON68, ISG, AFCI). To do this, experiments were conducted at temperatures of 23, 40, 70, and 90 °C and pH(RT) values of 9, 10, 11, and 12 with the single-pass flow-through (SPFT) test method. The results from these tests were then used to parameterize a kinetic rate model based on transition state theory. Both the absolute dissolution rates and the rate model parameters are compared with previous results. Discrepancies in the absolute dissolution rates as compared to those obtained using other test methods are discussed. Rate model parameters for the three glasses studied here are nearly equivalent within error and in relative agreement with previous studies. The results were analyzed with a linear multivariate regression (LMR) and a nonlinear multivariate regression performed with the use of the Glass Corrosion Modeling Tool (GCMT), which is capable of providing a robust uncertainty analysis. This robust analysis highlights the high degree of correlation of various parameters in the kinetic rate model. Asmore » more data are obtained on borosilicate glasses with varying compositions, the effect of glass composition on the rate parameter values could possibly be obtained. This would allow for the possibility of predicting the forward dissolution rate of glass based solely on composition« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1436843
Report Number(s):
PNNL-SA-126627
Journal ID: ISSN 0016-7037; AF5805010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Geochimica et Cosmochimica Acta; Journal Volume: 226; Journal Issue: C
Country of Publication:
United States
Language:
English

Citation Formats

Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., and Asmussen, R. Matthew. The dissolution behavior of borosilicate glasses in far-from equilibrium conditions. United States: N. p., 2018. Web. doi:10.1016/j.gca.2018.02.001.
Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., & Asmussen, R. Matthew. The dissolution behavior of borosilicate glasses in far-from equilibrium conditions. United States. doi:10.1016/j.gca.2018.02.001.
Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., and Asmussen, R. Matthew. Sun . "The dissolution behavior of borosilicate glasses in far-from equilibrium conditions". United States. doi:10.1016/j.gca.2018.02.001.
@article{osti_1436843,
title = {The dissolution behavior of borosilicate glasses in far-from equilibrium conditions},
author = {Neeway, James J. and Rieke, Peter C. and Parruzot, Benjamin P. and Ryan, Joseph V. and Asmussen, R. Matthew},
abstractNote = {In far-from-equilibrium conditions, the dissolution of borosilicate glasses used to immobilize nuclear waste is known to be a function of both temperature and pH. The aim of this paper is to study effects of these variables on three model waste glasses (SON68, ISG, AFCI). To do this, experiments were conducted at temperatures of 23, 40, 70, and 90 °C and pH(RT) values of 9, 10, 11, and 12 with the single-pass flow-through (SPFT) test method. The results from these tests were then used to parameterize a kinetic rate model based on transition state theory. Both the absolute dissolution rates and the rate model parameters are compared with previous results. Discrepancies in the absolute dissolution rates as compared to those obtained using other test methods are discussed. Rate model parameters for the three glasses studied here are nearly equivalent within error and in relative agreement with previous studies. The results were analyzed with a linear multivariate regression (LMR) and a nonlinear multivariate regression performed with the use of the Glass Corrosion Modeling Tool (GCMT), which is capable of providing a robust uncertainty analysis. This robust analysis highlights the high degree of correlation of various parameters in the kinetic rate model. As more data are obtained on borosilicate glasses with varying compositions, the effect of glass composition on the rate parameter values could possibly be obtained. This would allow for the possibility of predicting the forward dissolution rate of glass based solely on composition},
doi = {10.1016/j.gca.2018.02.001},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 226,
place = {United States},
year = {Sun Apr 01 00:00:00 EDT 2018},
month = {Sun Apr 01 00:00:00 EDT 2018}
}