Thermodynamic Approach for Predicting Actinide and Rare Earth Concentrations in Leachates from Radioactive Waste Glasses |
| |
Authors: | Dhanpat Rai Mikazu Yui Akira Kitamura Bernd Grambow |
| |
Institution: | (1) Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306-4390, USA |
| |
Abstract: | Studies aimed primarily at determining leach rates of different elements from doped glasses have resulted in computerized
models for predicting leachate concentrations. However, leach rate related data should be limited to predicting the stability
behavior of the glass matrix; the radionuclide release data based on these studies are empirical and are highly dependant
on many variables and processes which have not been systematically evaluated and thus do not provide a reliable method of
predicting leachate concentrations. A better approach is available for those elements that can readily form relatively insoluble
solids during preparation of glass or glass/water interactions. This alternate approach relies on the experimental solubilities
of pulverized doped glasses, in a wide range of well-controlled important variables such as pH and pe, and their comparisons
at the given aqueous composition to predicted solubilities of known solid phases from the thermodynamic data. These comparisons
are used to indirectly identify specific solubility-controlling solids in doped glass/water systems to determine scientifically
defensible aqueous concentrations of different elements for any given groundwater composition, independent of glass dissolution
kinetics and independent of time. This paper summarizes data available for the application of this alternate approach to reliably
predict concentrations of thorium, uranium, neptunium, plutonium, and trivalent actinides and rare earth elements leachable
from the doped glasses. The thermodynamic data, in addition to that reported in recent critical reviews, includes new data
that were developed for the solubility products of Th3(PO4)4(s) and the solid solutions of trivalent actinides and rare earth hydroxides. Thermodynamic interpretations of the doped glass
solubility data show specifically that tetravalent actinide hydrous/crystalline oxides and solid solutions of trivalent actinides
and rare earths hydroxides in non-phosphate glasses and Th3(PO4)4(s) and MPO4(s), where M denotes trivalent actinides or rare earths, in phosphate-containing glasses are the dominant solubility-controlling
solids. Needed future research in this area is briefly outlined. |
| |
Keywords: | |
本文献已被 SpringerLink 等数据库收录! |
|