Utilization of kinetic isotope effects for the concentration of tritium. 1998 annual progress report
'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 authors intend to develop a process to remove tritium from H{sub 2}O by concentrating it with respect to protio-water. This research involves developing chemical cycles that produce high concentration factors for HTO and T{sub 2}O 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.'
- Research Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Organization:
- USDOE Office of Environmental Management (EM), Office of Science and Risk Policy
- OSTI ID:
- 13744
- Report Number(s):
- EMSP-55103-98; ON: DE00013744
- Country of Publication:
- United States
- Language:
- English
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