【作者】 林子健； 林蕴良； 郭子方； 李一帆； 杜香怡； 林铭章；

【Author】 LIN Zi-jian;LIN Yun-liang;GUO Zi-fang;LI Yi-fan;DU Xiang-yi;LIN Ming-zhang;School of Nuclear Science and Technology,University of Science and Technology of China;

【机构】 中国科学技术大学核科学技术学院；

【摘要】 铜与铜合金广泛应用于核材料领域,对于材料腐蚀控制和氢爆风险评估,含铜离子水溶液辐解的影响必须予以考虑。本工作开展了含铜离子水溶液γ辐解实验,探究了不同吸收剂量、吸收剂量率和Cu²⁺浓度对H₂O₂、O₂和H2生成的影响。实验结果表明,随着吸收剂量的增加（0～1.80 kGy）,H₂O₂和气相中H₂的浓度先增大后趋于稳态,其稳态浓度分别为5.41×10^-6 mol/L和7.91×10^-5 mol/L,而气相中O₂的浓度则维持在9.04×10^-4 mol/L。Cu²⁺的存在使H₂、H₂O₂的平衡浓度分别提升一个和两个数量级,对H₂O₂、H₂的生成起到了促进作用,但对O₂的生成基本没有影响。H₂O₂和H₂的平衡浓度随着吸收剂量率的增大而升高,当吸收剂量率从1.40 Gy/min增大到46.93 Gy/min,其平衡浓度分别从4.56×10^-6 mol/L和1.78×10^-5 mol/L升高到2.46×10^-5 mol/L和3.81×10^-4 mol/L,而在此吸收剂量率范围内O2基本不受影响。同时,基于水辐解反应动力学和气液两相传质双膜理论,我们构建了含铜离子水溶液辐解计算模型。模拟结果与实验数据相比,标准化平均偏差的绝对值基本在1%～7%,最大约24%,证明了计算模型的有效性和正确性。更多还原

【Abstract】 Copper and copper alloys are widely used in the field of nuclear materials.The influence of copper ion containing aqueous solution radiolysis must be considered for material corrosion control and hydrogen explosion risk assessment.In this work,y-radiolysis experiment of aqueous solution containing copper ion was carried out to explore the effects of different absorbed doses,absorbed dose rates and Cu²⁺ concentrations on the generation of H₂ O₂,O₂ and H₂.The experimental results show that with the increase of absorbed dose（0～1.80 kGy）,the concentrations of H₂ O₂ and H₂（g） first increase and then tend to be stable,with steady-state concentrations of 5.41 × 10^-6 mol/L and 7.91×10^-5 mol/L,respectively, while the concentration of O₂（g） remains at 9.04×10^-4 mol/L.The presence of Cu²⁺ enhances the equilibrium concentrations of H₂ and H₂ O₂ by one and two orders of magnitude,respectively,which promotes the generation of H₂ O₂ and H₂ but has little effect on the generation of O₂.The equilibrium concentrations of H₂ O₂ and H₂ increase with increasing absorption dose rate,and when the absorption dose rate is increased from 1.40 Gy/min to 46.93 Gy/min,their equilibrium concentrations increase from 4.56 × 10^-6 mol/L and 1.78 × 10^-5 mol/L to 2.46 × 10^-5 mol/L and 3.81 ×10^-4 mol/L,respectively,while O₂ is basically unaffected within this absorption dose rate range.Meanwhile,based on the kinetics of water radiolysis and the two-film theory of gas-liquid mass transfer,we constructed a calculation model for the radiolysis of aqueous solution containing copper ion.Compared with experimental data,the absolute values of normalized mean bias in simulation results are generally between 1% and 7%,with a maximum of about 24%,demonstrating the effectiveness and correctness of the calculation model.更多还原