Utilization of Kinetic Isotope Effects for the Concentration of Tritium

[摘要] The objective of this project was the development of methods for concentrating tritium in water based on large primary isotope effects in catalytic redox processes. Basic research was conducted to develop the chemistry of a complete cyclic process. 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 could be incorporated in an organic polymer or other solid waste form which will prevent its ready transport in ground water. The research was aimed at developing chemical cycles that produce high concentration factors for HTO and T2O. H-T discrimination occurs in an oxidation step involving a transition metal oxidant and small organic compounds containing oxidizable C-H or C-T bonds. Strong primary kinetic isotope effects lead to preferential oxidation of C-H bonds whose products are readily removed from the unreacted C-T compound. Since the reduced transition metal oxidant may be easily regenerated in an electrochemical reaction, the oxidation of the organic substrate becomes catalytic. On the other side of the cycle, tritium in the form of HTO and T2O is incorporated into the oxidized organic substrate in a reductive process, and thus the chemical cycle may be closed.

[发布日期] 2001-12-31 [发布机构] Oak Ridge National Laboratory

[关键词] Organic Compounds;Tritium;Ground Water;Water;37 Inorganic, Organic, Physical And Analytical Chemistry