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Skomurski, Frances N.

Publications and source records attributed to Skomurski, Frances N..

Experimental Results for SimFuels

Assessing the performance of Spent (or Used) Nuclear Fuel (UNF) 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 UO 2 , 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 that may increase the waste form degradation rate and change radionuclide behavior. To study UNF, we have been working on producing synthetic UO 2 ceramics, or SimFuels that can be used in testing and which will contain specific radionuclides or non-radioactive analogs so that we can test the impact of radiolysis on fuel corrosion without using actual spent fuel. Although, testing actual UNF would be ideal for understanding the long term behavior of UNF, it requires the use of hot cells and is extremely expensive. In this report, we discuss, factors influencing the preparation of SimFuels and the requirements for dopants to mimic the behavior of UNF. We have developed a reliable procedure for producing large grain UO 2 at moderate temperatures. This process will be applied to a series of different formulations.

Geological Disposal↗

Radiolysis Process Model

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 UO 2 , 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, O 2 -, eaq, H 2 O 2 , H 2 , and O 2 ) that may increase the waste form degradation rate and change radionuclide behavior. H 2 O 2 is the dominant oxidant for spent nuclear fuel in an O 2 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 [H 2 O 2 ] 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.

Hydrogen Peroxide↗