含铜离子水溶液的辐射分解行为  

Radiolysis of aqueous solution containing copper ions

作　　者：林蕴良 郭子方 林子健 吴志豪 周煜筑 张鹏 林铭章[1] LIN Yunliang;GUO Zifang;LIN Zijian;WU Zhihao;ZHOU Yuzhu;ZHANG Peng;LIN Mingzhang(School of Nuclear Science and Technology,University of Science and Technology of China,Hefei 230026,China;National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China)

机构地区：[1]中国科学技术大学核科学技术学院,合肥230026 [2]中国科学技术大学国家同步辐射实验室,合肥230029

出　　处：《辐射研究与辐射工艺学报》2023年第4期1-10,共10页Journal of Radiation Research and Radiation Processing

基　　金：国家自然科学基金“叶企孙”科学基金(U2241289)资助。

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Cu^(2+)浓度对H_(2)O_(2)、O_(2)和H_(2)生成的影响。实验结果表明:随着吸收剂量的增加(0~1.80 kGy),H_(2)O_(2)和气相中H_(2)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O_(2)的浓度则维持在9.04×10^(-4)mol/L。Cu^(2+)的存在使H_(2)、H_(2)O_(2)的平衡浓度分别提升一个和两个数量级,对H_(2)O_(2)、H_(2)的生成起到促进作用,但对O_(2)的生成基本没有影响。H_(2)O_(2)和H_(2)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O_(2)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%之间,最大约24%,证明了计算模型的有效性和正确性。在此基础上,运用该模型计算了C^(6+)离子辐照下含铜离子水溶液的辐解行为,模拟结果与文献报道的实验数据吻合良好,表明模型具备可扩展性。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 H_(2)O_(2),O_(2),and H_(2)must be considered for material corrosion control and hydrogen explosion risk assessment.In this study,aγ-radiolysis experiment of an aqueous solution containing copper ions was conducted to explore the effects of different absorbed doses,absorption dose rates,and Cu^(2+)concentrations on the generation of H_(2)O_(2),O_(2),and H_(2).The results showed that with an increase in the absorbed dose(0−1.80 kGy),the concentrations of H_(2)O_(2)and H_(2)(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 O_(2)(g)remained at 9.04×10^(-4)mol/L.The presence of Cu^(2+)enhanced the equilibrium concentrations of H_(2)and H_(2)O_(2)by one and two orders of magnitude,respectively,which in turn promoted the generation of H_(2)O_(2)and H_(2);however,it had a negligible effect on O_(2)generation.The equilibrium concentrations of H_(2)O_(2)and H_(2)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 H_(2)O_(2)and H_(2)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 O_(2)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 radiolyti

关 键 词：含铜离子水溶液 Γ射线 辐射分解 化学动力学模拟 

分 类 号：TL13[核科学技术—核能科学]