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Effects of Iron and pH on Glass Dissolution Rate

Published online by Cambridge University Press:  11 February 2011

Seung-Young Jeong
Affiliation:
Chemical Technology Division, Argonne National Laboratory, 9700 S. Cass Ave. Argonne, IL 60439
William L. Ebert
Affiliation:
Chemical Technology Division, Argonne National Laboratory, 9700 S. Cass Ave. Argonne, IL 60439
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Abstract

Short-term static tests were conducted with a surrogate high-level waste glass to measure the effects of pH and dissolved iron on the glass dissolution rate. The tests were conducted to determine if a term to account for the effects of dissolved iron is needed in the glass degradation model developed for Total System Performance Assessment (TSPA) calculations for the Yucca Mountain disposal system license application. The glass degradation model includes terms for dependencies on temperature, pH, and chemical affinity. A series of tests was conducted at 90 °C in various pH solutions without iron and with added FeCl3, Fe2O3, Fe3O4, and FeOOH. Tests were conducted at glass surface area/solution volume (S/V) ratios about 2 and 10 m-1 for between 2 and 21 days. Solution concentrations of boron were used to measure the extent of reaction and calculate the glass dissolution rates. Similar rates were measured in tests conducted with and without iron at each pH. Both the results of the tests with and without iron showed V-shaped pH dependence curves with minima at near-neutral pH values. The pH dependencies (η) are about 0.44 in basic solutions and –0.49 in acidic solutions, based on the combined results of tests with and without iron. These are within the range of values for the pH dependence in the TSPA model for site recommendation.

Type
Research Article
Copyright
Copyright © Materials Research Society 2003

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