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ISSN Online: 2379-1748

7th Thermal and Fluids Engineering Conference (TFEC)
SJR: 0.152 SNIP: 0.14 CiteScore™:: 0.5

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Clarivate CPCI (Proceedings) Scopus
May, 15-18, 2022 , Las Vegas, NV, USA

AN EXPERIMENTAL AND MODELING STUDY OF OXIDATION OF HYDROGEN ISOTOPES AT TRACE CONCENTRATIONS

Get access (open in a dialog) pages 1421-1432
DOI: 10.1615/TFEC2022.cbf-ii.040826

Abstract

In accident scenarios involving release of tritium during handling and storage, the level of risk to human health is dominated by the extent to which radioactive tritium is oxidized to the water form (T2O or THO). At some facilities, tritium inventories consist of very small quantities stored at sub-atmospheric pressure, which means that tritium release accident scenarios will likely produce concentrations in air that are well below the lower flammability limit. It is known that isotope effects on reaction rates should result in slower oxidation rates for heavier isotopes of hydrogen, but this effect has not previously been quantified for oxidation at concentrations well below the lower flammability limit for hydrogen. This work describes hydrogen isotope oxidation measurements in an atmospheric tube furnace reactor. These measurements consist of five concentration levels between 0.01% and 1% protium or deuterium and two residence times. Oxidation is observed to occur between about 550°C and 800°C, with higher levels of conversion achieved at lower temperatures for protium with respect to deuterium at the same volumetric inlet concentration and residence time. Computational fluid dynamics simulations of the experiments were used to customize reaction orders and Arrhenius parameters in a 1-step oxidation mechanism. The trends in the rates for protium and deuterium are extrapolated based on guidance from literature to produce kinetic rate parameters appropriate for tritium oxidation at low concentrations.