Radiolysis Process Model

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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, ... continued below

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Buck, Edgar C.; Wittman, Richard S.; Skomurski, Frances N.; Cantrell, Kirk J.; McNamara, Bruce K. & Soderquist, Chuck Z. July 17, 2012.

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Description

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.

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  • Report No.: PNNL-21554
  • Grant Number: AC05-76RL01830
  • DOI: 10.2172/1069211 | External Link
  • Office of Scientific & Technical Information Report Number: 1069211
  • Archival Resource Key: ark:/67531/metadc834915

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Office of Scientific & Technical Information Technical Reports

Reports, articles and other documents harvested from the Office of Scientific and Technical Information.

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  • July 17, 2012

Added to The UNT Digital Library

  • May 19, 2016, 9:45 a.m.

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  • Dec. 9, 2016, 6:55 p.m.

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Buck, Edgar C.; Wittman, Richard S.; Skomurski, Frances N.; Cantrell, Kirk J.; McNamara, Bruce K. & Soderquist, Chuck Z. Radiolysis Process Model, report, July 17, 2012; Richland, Washington. (digital.library.unt.edu/ark:/67531/metadc834915/: accessed May 24, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.