Differential Scanning Calorimetry of Metamict Pu-Substituted Zirconolite

Abstract

ABSTRACTSamples of CaPuTi2O7 were prepared by cold pressing and sintering. Plutonium was substituted for zirconium in order to characterize radiation damage effects. The energy stored in a sample which had reached saturation in swelling after storage at ambient temperature was measured with a differential scanning calorimeter. The total energy of 6.6±0.1 cal/g is released over the range 485–715° C. The activation energy of annealing of the damage is 1.22±0.05 eV. The temperature dependence of the rate constant is described by kT= 5.96E4 exp(−1.22/kBT) s−1 where kB and T are the Boltzmann's constant and temperature(K) respectively. A sample stored at 600°C was similarly evaluated and showed no release of stored energy to the precision of the apparatus (±0.1 cal/g). These results are applied to analysis of waste incorporation in Synroc and are correlated with analogous parameters for other materials.