“Trapped fraction” effect in microfuel with plutonium fuel

Results of the investigation into the thermodynamics of two types of microfuel (with oxygen getter and without it) with plutonium fuel for various degrees of burnup are presented. The behavior of the trapped fraction of Ag, Ce, Cd, Cs, La, Mo, Pu, Pd, Ru, Sr, Te, and Y is investigated. The fraction of any fission product bound into stable chemical compounds with other components of the system and excluded from the diffusion process is called the trapped fraction. An abrupt increase in the trapped fraction of cesium and, correspondingly, a decrease in free cesium during the burnup of ～26% FIMA (fissions per initial metal atom) or more are found for the microfuel containing no oxygen getter. This leads to a substantial nonlinear burnup dependence of the trapped fraction and should be the cause of an abrupt decrease in the Cs output from the microfuel. It seems likely that the found effect is associated with the formation of carbonate Cs₂CO₃ in the plutonium fuel. In the case of microfuel containing the oxygen getter, no formation of cesium carbonate occurs and the trapped fraction of cesium is almost independent of the burnup.     

Some Thermodynamic Features of Uranium–Plutonium Nitride Fuel in the Course of Burnup

Calculation studies on the effect of carbon and oxygen impurities on the chemical and phase compositions of nitride uranium–plutonium fuel in the course of burnup are performed using the IVTANTHERMO code. It is shown that the number of moles of UN decreases with increasing burnup level, whereas UN_1.466, UN_1.54, and UN_1.73 exhibit a considerable increase. The presence of oxygen and carbon impurities causes an increase in the content of the UN_1.466, UN_1.54 and UN_1.73 phases in the initial fuel by several orders of magnitude, in particular, at a relatively low temperature. At the same time, the presence of impurities abruptly reduces the content of free uranium in unburned fuel. Plutonium in the considered system is contained in form of Pu, PuC, PuC₂, Pu₂C₃, and PuN. Plutonium carbides, as well as uranium carbides, are formed in small amounts. Most of the plutonium remains in the form of nitride PuN, whereas unbound Pu is present only in the areas with a low burnup level and high temperatures.     

Simulation of Fission Product Release from Microfuel Particles Taking into Account the Effects of Trapped Fraction and Concentration Jumps at the Interfaces

A modification of the FP Kinetics code [1] has been performed to calculate the fission product release from HTGR microfuel particles, allowing for chemical binding, limited solubility effects, and component concentration jumps at the interfaces of the coating layers. A comparison is made of the release curves of Cs from microfuel particles calculated using the FP Kinetics and PARFUME codes [2]. It is shown that taking into account the concentration jumps at the interfaces of the silicon carbide layer makes it possible to give a noncontradictory explanation of the experimental data obtained for Cs release in post-reactor thermal testing. The need for performing experiments to determine the limits of solubility in coating materials is noted.

     

Analysis of the Range of Applicability of Thermodynamic Calculations in the Engineering of Nitride Fuel Elements

The domains of applicability of thermodynamic calculations in the engineering of nitride fuel are analyzed. Characteristic values of the following parameters, which affect directly the concentration equilibration time, are estimated: nuclide production rate; characteristic times to local equilibrium in the considered temperature range; characteristic time needed for a stationary temperature profile to be established; characteristic time needed for a quasi-stationary concentration field to be established on a scale comparable to the size of a fuel pellet. It is demonstrated that equilibrium thermodynamic calculations are suitable for estimating the chemical and phase composition of fuel. However, a two-layer kinetic model should be developed in order to characterize the transport processes in condensed and gaseous phases. The process of diffusive transport needs to be taken into account in order to determine the composition in the hot region at the center of a fuel element.