含铜离子水溶液的辐射分解行为

林蕴良; 郭子方; 林子健; 吴志豪; 周煜筑; 张鹏; 林铭章

doi:10.11889/j.1000-3436.2023-0006

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含铜离子水溶液的辐射分解行为

辐射化学 | 更新时间：2023-08-29

- 含铜离子水溶液的辐射分解行为
  封面论文
- Radiolysis of aqueous solution containing copper ions
- 辐射研究与辐射工艺学报 2023年41卷第4期页码：40201
- 作者机构：
  
  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
- 作者简介：
  
  林蕴良，男，1997年7月出生，2020年6月于中国科学技术大学获学士学位，目前为中国科学技术大学在读硕士研究生，核科学与技术专业
  林铭章，教授，博士生导师，E-mail: gelin@ustc.edu.cn
- 基金信息：
  
  国家自然科学基金“叶企孙”科学基金(U2241289)
- DOI：10.11889/j.1000-3436.2023-0006
  中图分类号：
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林蕴良, 郭子方, 林子健, 等. 含铜离子水溶液的辐射分解行为[J]. 辐射研究与辐射工艺学报, 2023,41(4):040201.

LIN Yunliang, GUO Zifang, LIN Zijian, et al. Radiolysis of aqueous solution containing copper ions[J]. Journal of Radiation Research and Radiation Processing, 2023,41(4):040201.
林蕴良, 郭子方, 林子健, 等. 含铜离子水溶液的辐射分解行为[J]. 辐射研究与辐射工艺学报, 2023,41(4):040201. DOI： 10.11889/j.1000-3436.2023-0006.

LIN Yunliang, GUO Zifang, LIN Zijian, et al. Radiolysis of aqueous solution containing copper ions[J]. Journal of Radiation Research and Radiation Processing, 2023,41(4):040201. DOI： 10.11889/j.1000-3436.2023-0006.

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。

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 H,2,O,2, O,2, and H,2, 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 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 radiolytic behavior of an aqueous solution containing copper ions under C,6+, 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.

关键词

含铜离子水溶液γ射线辐射分解化学动力学模拟

Keywords

Aqueous solution containing copper ionγ-raysRadiolysisChemical kinetics modeling

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