Radiolysis of aqueous solution containing copper ions

Abstract

Copper and copper alloys are widely used in the field of nuclear materials. The effects of aqueous solutions that have undergone copper ion radiolysis on the generation of H2O2, O2, and H2 must be considered for material corrosion control and hydrogen explosion risk assessment. In this study, a γ-radiolysis experiment of an aqueous solution containing copper ions was conducted to explore the effects of different absorbed doses, absorption dose rates, and Cu2+ concentrations on the generation of H2O2, O2, and H2. The results showed that with an increase in the absorbed dose (0-1.80 kGy), the concentrations of H2O2 and H2(g) firstly increased and then tended to stabilize under steady-state concentrations of 5.41×10-6 and 7.91×10-5 mol/L, respectively, whereas the concentration of O2(g) remained at 9.04×10-4 mol/L. The presence of Cu2+ enhanced the equilibrium concentrations of H2 and H2O2 by one and two orders of magnitude, respectively, which in turn promoted the generation of H2O2 and H2; however, it had a negligible effect on O2 generation. The equilibrium concentrations of H2O2 and H2 increased with an increase in the absorption dose rate. Specifically, when the absorption dose rate was increased from 1.40 to 46.93 Gy/min, the equilibrium concentrations of H2O2 and H2 increased from 4.56×10-6 and 1.78×10-5 mol/L to 2.46×10-5 and 3.81×10-4 mol/L, respectively, whereas O2 remained essentially unaffected within this absorption dose rate range. In addition, based on the kinetics of water radiolysis and two-film theory of gas-liquid mass transfer, we constructed a calculation model for the radiolysis of aqueous solutions containing copper ions. Compared with the experimental data, the absolute values of the normalized mean bias in the simulation results were mostly between 1% and 7%, with a maximum of approximately 24%, thereby demonstrating the effectiveness and correctness of the calculation model. Accordingly, the model was used to calculate the radiolytic behavior of an aqueous solution containing copper ions under C6+ ion irradiation, and the simulation results matched well with the experimental data reported in the literature, indicating that the model can be expanded to other applications.

Keywords

• aqueous solution containing copper ion
• γ-rays
• radiolysis
• chemical kinetics modeling