Monte-Carlo Simulation of &gamma;-ray and Fast Neutron Radiolysis of Liquid Water and 0.4 <em>M</em> H₂SO₄ Solutions at Temperatures up to 325^oC

Abstract

Monte-Carlo simulations were used to study the radiolysis of liquid water at ο C when subjected to low linear energy transfer (LET) of 60 Co γ-ray radiation and fast neutrons of 2 and 0.8 MeV. The energy deposited in the early stage of 60 Co γ-ray irradiation was approximated by considering short segments (~150 µm) of 300 MeV proton tracks, corresponding to an average LET of ~0.3 keV/µm. In case of 2 MeV fast neutrons, the energy deposited was considered by using short segments (~5 µm) of energy at 1.264, 0.465, 0.171, 0.063 and 0.24 MeV. 0.8 MeV fast neutrons were approximated by 0.505, 0.186, 0.069 and 0.025 MeV protons. The effect of 0.4 M H 2 SO 4 solution on radiolysis was also studied by this method for both 60 Co γ-rays and 0.8 MeV fast neutrons. The simulated results at the time of 10 -7 s after irradiation were obtained and compared with the available experimental results published by other researchers to be in excellent agreement with them over the entire temperature ranges and radiation sources studied. Except for g(H 2 ) that increase with temperature rises, the general behaviors of higher radical products and lower molecular products at higher temperatures were obtained. The LET effect is also validated by this study, showing that the increase in LET would yield higher molecular and lower radical products. Studies on 0.4 M H 2 SO 4 solutions also show good agreement between the computed and experimental data for γ-ray irrradiation: the presence of 0.4 M H + , except for g(H 2 ) that gives lower value at 25 ο C and higher value at 325 ο C, gives the higher values for radicals and g(H 2 O 2 ) at 25 ο C and lower values at 325 ο C, compared with that for neutral water. The computed data show good agreement with the experimental data for 0.4 M H 2 SO 4 solutions induced by 0.8 MeV fast neutrons, except for g(H 2 ) and g(H •) that gives good agreement up to 50 ο C, then the opposite tendencies with the further temperature rises. However, the simulated fast neutron radiolysis on acidic demonstrates similar tendencies on temperature dependence with that for simulated 60 Co γ-radiolysis, but in different magnitude. For better understanding, more experimental data for fast neutrons are needed, especially under the acidic conditions.

Temperature Dependence of the Primary Species Yields of Liquid Water Radiolysis by 0.8-MeV Fast Neutrons

“…As the LET of the radiation increases (the less the energy), many radical interactions occurred therefore the higher the yield of molecular products. Also, we compared our present work with the work of Sunaryo et al [6], but at this time we used the information available at [7] in the code. Indeed, Sunaryo et al did not take into account the reaction rate constant of the two reactions discussed previously.…”

“…Peculiarly, there are limited data of the fast neutron G-values in the literature as compared to the gamma ones, especially at high temperatures. However, Sunaryo et al [6] have simulated this energy at the temperature range of 25-325°C. Furthermore, there is much updated information which has been incorporated in the code developed by J.-P. Jay-Gerin's group in Université de Sherbrooke, Québec, Canada as follows.…”

Boric Acid Radiolysis in Primary Coolant Water of PWR at Temperature of 250oC

“…The simulation method has been reported elsewhere [5,[9][10][11][12][13][14]. Radiolysis simulation is an analysis of simultaneous chemical reactions and the integration of time-dependent multivariable simultaneous differential equations.…”

“…eaq-+ H + H2O = H2 + OH -2.76x10 10 4.97 x10 11 3. eaq-+ OH = OH -3.50x10 10 3.73 x10 11 4. eaq-+ H2O2 = OH + OH -1.40x10 10 3.85 x10 11 5. eaq-+ O2 = O2 -2.30 x10 10 2.18 x10 11 6. eaq-+ O2 -+ 2H2O = H2O2 + 2OH -1.30 x10 10 1.61 x10 11 7. eaq-+ HO2 = HO2 -1.28 x10 10 1.61 x10 11 8. H + H = H2 5.14 x10 9 1.04 x10 11 9. H + OH = H2O 1.10 x10 10 6.34 x10 10…”