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Radiochimica Acta

International Journal for chemical aspects of nuclear science and technology

Ed. by Qaim, Syed M.

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Use of thermodynamic sorption models to derive radionuclide Kd values for performance assessment: selected results and recommendations of the NEA sorption project

Michael Ochs / James A. Davis / Markus Olin / Timothy E. Payne / Cherry J. Tweed / M. M. Askarieh / S. Altmann

Citation Information: Radiochimica Acta. Volume 94, Issue 9-11, Pages 779–785, ISSN (Print) 0033-8230, DOI: 10.1524/ract.2006.94.9-11.779, September 2009

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For the safe final disposal and/or long-term storage of radioactive wastes, deep or near-surface underground repositories are being considered world-wide. A central safety feature is the prevention, or sufficient retardation, of radionuclide (RN) migration to the biosphere. To this end, radionuclide sorption is one of the most important processes. Decreasing the uncertainty in radionuclide sorption may contribute significantly to reducing the overall uncertainty of a performance assessment (PA).

For PA, sorption is typically characterised by distribution coefficients (Kd values). The conditional nature of Kd requires different estimates of this parameter for each set of geochemical conditions of potential relevance in a RN´s migration pathway. As it is not feasible to measure sorption for every set of conditions, the derivation of Kd for PA must rely on data derived from representative model systems. As a result, uncertainty in Kd is largely caused by the need to derive values for conditions not explicitly addressed in experiments.

The recently concluded NEA Sorption Project [1] showed that thermodynamic sorption models (TSMs) are uniquely suited to derive Kd as a function of conditions, because they allow a direct coupling of sorption with variable solution chemistry and mineralogy in a thermodynamic framework. The results of the project enable assessment of the suitability of various TSM approaches for PA-relevant applications as well as of the potential and limitations of TSMs to model RN sorption in complex systems.

Keywords: Radioactive waste; Sorption models; Kd value; Uncertainty; Surface complexation

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