Radiolysis Process Model

Buck, Edgar C. ; Wittman, Richard S. ; Skomurski, Frances N. ; Cantrell, Kirk J. ; McNamara, Bruce K. ; Soderquist, Chuck Z.

关键词: used fuel;    spent nuclear fuel;    radiolysis;    uranium;    hydrogen peroxide;   

DOI  :  10.2172/1069211
RP-ID  :  PNNL-21554
PID  :  OSTI ID: 1069211
Others  :  Other: AF5865010

美国|英语

来源: SciTech Connect

【 摘 要 】

Assessing the performance of spent (used) nuclear fuel in geological repository requires quantification of time-dependent phenomena that may influence its behavior on a time-scale up to millions of years. A high-level waste repository environment will be a dynamic redox system because of the time-dependent generation of radiolytic oxidants and reductants and the corrosion of Fe-bearing canister materials. One major difference between used fuel and natural analogues, including unirradiated UO2, is the intense radiolytic field. The radiation emitted by used fuel can produce radiolysis products in the presence of water vapor or a thin-film of water (including OH??? and H??? radicals, O2-, eaq, H2O2, H2, and O2) that may increase the waste form degradation rate and change radionuclide behavior. H2O2 is the dominant oxidant for spent nuclear fuel in an O2 depleted water environment, the most sensitive parameters have been identified with respect to predictions of a radiolysis model under typical conditions. As compared with the full model with about 100 reactions it was found that only 30-40 of the reactions are required to determine [H2O2] to one part in 10???5 and to preserve most of the predictions for major species. This allows a systematic approach for model simplification and offers guidance in designing experiments for validation.