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Chemical thermodynamics of actinide coordination in solution at variable temperatures

The temperature in the nuclear waste storage tanks and in the vicinity of high-level nuclear wastes in the repository could be significantly higher than 25 o C due to the decay energy of radioactive materials. Thus, reliable models for predicting the chemical behavior of actinides in the waste processing and in the “near-field” environment must properly take into consideration the temperature effect on the coordination of actinides with ligands that may be present. Currently, very few data are available on the coordination of actinides at elevated temperatures. The approximation methods, including the “constant enthalpy” approach, the “constant heat capacity” approach, the DQUANT equation and the revised HFK equation, have not been extensively tested because of the lack of experimental data. To extend the thermodynamic database to include the effect of temperature on the coordination of actinides, a research program has been started at Lawrence Berkeley National Laboratory to investigate the coordination of actinides in solution at variable temperatures.