caa a22 4500 445328479 CHVBK 20180317142729.0 cr unu---uuuuu 170323e20110901xx s 000 0 eng 10.1007/s10953-011-9725-z doi (NATIONALLICENCE)springer-10.1007/s10953-011-9725-z Thermodynamic Approach for Predicting Actinide and Rare Earth Concentrations in Leachates from Radioactive Waste Glasses [Elektronische Daten] [Dhanpat Rai, Mikazu Yui, Akira Kitamura, Bernd Grambow] 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. Springer Science+Business Media, LLC, 2011 Solubility nationallicence Solubility-controlling solids nationallicence Glass dissolution nationallicence Radioactive glass nationallicence Thorium nationallicence Uranium nationallicence Neptunium nationallicence Plutonium nationallicence Neodymium nationallicence Rare earths nationallicence Rai Dhanpat Rai Enviro-Chem, P.O. Box 784, Yachats, OR, USA aut Yui Mikazu Japan Atomic Energy Agency, Tokai, Japan aut Kitamura Akira Japan Atomic Energy Agency, Tokai, Japan aut Grambow Bernd SUBATECH/Ecole des Mines de Nantes, Université de Nantes IN2P3/CNRS, Nantes, France aut Journal of Solution Chemistry Springer US; http://www.springer-ny.com 40/8(2011-09-01), 1473-1504 0095-9782 40:8<1473 2011 40 10953 https://doi.org/10.1007/s10953-011-9725-z text/html Onlinezugriff via DOI 1 research-article jats NATIONALLICENCE 856 40 https://doi.org/10.1007/s10953-011-9725-z text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Rai Dhanpat Rai Enviro-Chem, P.O. Box 784, Yachats, OR, USA aut NATIONALLICENCE 700 1- Yui Mikazu Japan Atomic Energy Agency, Tokai, Japan aut NATIONALLICENCE 700 1- Kitamura Akira Japan Atomic Energy Agency, Tokai, Japan aut NATIONALLICENCE 700 1- Grambow Bernd SUBATECH/Ecole des Mines de Nantes, Université de Nantes IN2P3/CNRS, Nantes, France aut NATIONALLICENCE 773 0- Journal of Solution Chemistry Springer US; http://www.springer-ny.com 40/8(2011-09-01), 1473-1504 0095-9782 40:8<1473 2011 40 10953 Metadata rights reserved Springer special CC-BY-NC licence nationallicence BK010053 XK010053 XK010000 NATIONALLICENCE NATIONALLICENCE NL-springer