Studies on nucleation and crystal growth kinetics of uranium(IV) oxalate

An improved apparatus is used for nucleation measurements according to Nielsen’s method. A new method is proposed to calculate the dilution ratio N of the reaction solution during nucleation rate determination. With the rule, when the initial apparent supersaturation ratio S′ = f(N) in the dilution tank is controlled from 1.2 to 2.7, crystal nucleus dissolving and secondary nucleation can be avoided satisfactorily. Experiments are realized by varying the supersaturation ratio from 26.0 to 297.5 and temperature from 30 °C to 50 °C. Uranium(IV) oxalate is precipitated by mixing equal volumes of tetravalent uranium nitrate and oxalic acid solution. The experimental results show that the nucleation rate of uranium(IV) oxalate in the supersaturation range as show above is characterized by the primary homogeneous mechanism and can be expressed by the equation ${R_N} = {A_N}{\rm{exp}}( - {E_a}/RT){\rm{exp}}[ - B/{({\rm{ln }}S)^2}],$ where AN = 1.9 × 1027 m−3s−1, Ea = 71.2 kJ mol−1, and B = 34.3. The crystal growth rate can be expressed by the equation $G(t) = {k_g}{\rm{exp(}} - {E^{\prime}_a}/RT{\rm{)(}}c - {c_{{\rm{eq}}}}{{\rm{)}}^g},$ where kg = 7.1 × 105 (mol/L)−0.98 (m/s), ${E^{\prime}_a} = 33.1 \ {\rm{ kJ \ mo}}{{\rm{l}}^{ - 1}},$ and g = 0.98. The results indicate that the crystal growth of tetravalent uranium(IV) oxalate is controlled by the BCF model.

Safety Analysis of Gas Pressure in a Subcritical Assembly for Molybdenum-99 Production System

The Subcritical Assembly for Molybdenum-99 Production system is a subcritical system fueled by uranium nitrate, which utilizes the Kartini reactor’s beam port as the neutron source. One of the problems in using uranium nitrate fuel involves the radiolysis reactions and gaseous fission products that form in the cavity above the Subcritical Assembly for Molybdenum-99 Production fuel tube, resulting in a buildup of pressure. To address this issue, this study examined the total accumulated gas pressure in each Subcritical Assembly for Molybdenum-99 Production tube contributed by gaseous fission products and water radiolysis by neutron and gamma radiation during 7 days of operation. Examinations were performed by combining the Subcritical Assembly for Molybdenum-99 Production and Kartini reactor geometry to obtain the burnup power using a tally within the Monte Carlo N-Particle eXtended code. Subcritical Assembly for Molybdenum-99 Production system was then simulated for 7 days with the obtained burnup power with the same code. Outputs from the code were then calculated and analyzed to determine the total accumulated pressure on each fuel tube from each of the pressure contributors. This research showed that the maximum accumulated pressures were 0.45 atm and 0.5 atm for Kartini reactor’s power of 100 kW and 110 kW, respectively. These pressures are lower than the atmospheric pressure; hence, the current Subcritical Assembly for Molybdenum-99 Production system can be operated safely for 7 days.