Utilization of Kinetic Isotope Effects for the Concentration of Tritium

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The objective of this research program is to develop methods for concentrating tritium in water based on large primary isotope effects in catalytic redox processes. Basic research is being conducted to develop the chemistry of a complete cyclic process. Because tritium (generally present as HTO) is in a rapidly established equilibrium with protio-water, it moves with groundwater and separation from water cannot be achieved by the usual pump-and-treat methods using sorbants. The general methodology developed in this work will be applicable to a number of DOE waste streams, and as a consequence of the process tritium will be incorporated into ... continued below

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Brown, Gilbert M.; Meyer, Thomas j. & Moyer, Bruce A. June 1, 1999.

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Description

The objective of this research program is to develop methods for concentrating tritium in water based on large primary isotope effects in catalytic redox processes. Basic research is being conducted to develop the chemistry of a complete cyclic process. Because tritium (generally present as HTO) is in a rapidly established equilibrium with protio-water, it moves with groundwater and separation from water cannot be achieved by the usual pump-and-treat methods using sorbants. The general methodology developed in this work will be applicable to a number of DOE waste streams, and as a consequence of the process tritium will be incorporated into an organic compound that will not readily exchange the tritium with groundwater. The process to be developed will remove tritium from H2O by concentrating it with respect to protio-water. This research involves developing chemical cycles that produce high concentration factors for HTO and T2O based on the discrimination of C-H and C-T bonds in oxidation reactions. Several steps are required in a cyclic process for the concentration of tritium in water. In the first step the tritium is incorporated in an organic compound. H-T discrimination occurs as the tritium containing compound is oxidized in a step involving a Ru(IV) oxo complex. Strong primary kinetic isotope effects lead to the oxidation of C-H bonds in preference to C-T bonds, and this reaction leads to concentration of tritium in the organic compound. The reduced form of the ruthenium compound can be reoxidized so that the oxidation step can be made catalytic.

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  • Other Information: PBD: 1 Jun 1999

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  • Report No.: EMSP-55103--1999
  • DOI: 10.2172/827393 | External Link
  • Office of Scientific & Technical Information Report Number: 827393
  • Archival Resource Key: ark:/67531/metadc786479

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  • June 1, 1999

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  • Dec. 3, 2015, 9:30 a.m.

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  • April 21, 2016, 4:27 p.m.

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Brown, Gilbert M.; Meyer, Thomas j. & Moyer, Bruce A. Utilization of Kinetic Isotope Effects for the Concentration of Tritium, report, June 1, 1999; United States. (digital.library.unt.edu/ark:/67531/metadc786479/: accessed August 18, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.