用于压水堆一回路去污的Ce（Ⅳ）+超声去污技术研究

摘要/Abstract

摘要： 针对压水堆一回路运行过程中生成的腐蚀产物,开展Ce（Ⅳ）加超声协同去污技术研究。选用304不锈钢作为样片,利用高压反应釜模拟压水堆一回路的腐蚀环境,制作出用于去污的腐蚀样片。探究不同的Ce（Ⅳ）浓度、硝酸浓度以及超声因素对去污效率的影响,研究不同条件下的去污液对金属基体材料的腐蚀情况。结果表明：高压反应釜制作出的腐蚀层表面形貌致密均匀,无明显的空洞开裂。去污实验中,Ce（Ⅳ）浓度对去污效果影响显著,当硝酸铈铵浓度为25 mmol/L时,去污液对氧化膜的去污效率最高;硝酸浓度对去污效果的影响并不显著,不同硝酸浓度下去污效率相差不大,但随着硝酸浓度的增加,去污效率呈现先上升后下降的趋势,当硝酸浓度为1.5 mol/L时去污效率达到最高;超声因素的加入会使去污效果显著提高;去污液与金属基体材料的相容性好,金属基体材料的腐蚀量最大为6.25 g/m²,远低于行业标准中规定的基体材料腐蚀量上限和精密部件腐蚀量上限。

关键词: 金属腐蚀, Ce（Ⅳ）去污, 超声去污

Abstract: Aiming at the corrosion products generated during the operation of the primary circuit of the pressurized water reactor, the synergistic decontamination technology of Ce(Ⅳ) and ultrasound was studied. The 304 stainless steel was selected as the sample, and the high-pressure reaction vessel was used to simulate the corrosion environment of the primary circuit of the pressurized water reactor to produce a corrosion sample for decontamination. The effects of different Ce(Ⅳ) concentration, nitric acid concentration and ultrasonic factors on the decontamination efficiency were investigated, and the corrosion of metal matrix materials under different conditions was studied. The results show that the surface morphology of the corrosion layer produced by the high-pressure reaction vessel is dense and uniform, and there are no obvious voids and cracks. In the decontamination experiment, the concentration of Ce(Ⅳ) has a significant impact on the decontamination effect. When the concentration of cerium ammonium nitrate is 25 mmol/L, the decontamination solution has the highest decontamination efficiency on the oxide film; The effect of nitric acid concentration on the decontamination effect is not significant, and the decontamination efficiency is not much different under different nitric acid concentrations. However, with the increase of nitric acid concentration, the decontamination efficiency increases first and then decreases. When the concentration of nitric acid is 1.5 mol/L, the decontamination efficiency reaches the highest; The addition of ultrasonic factors will significantly improve the decontamination effect; The decontamination solution has good compatibility with the metal matrix material; The maximum corrosion amount of the metal matrix material is 6.25 g/m², which is far lower than the upper limit of the corrosion amount of the matrix material and the upper limit of the corrosion amount of the precision parts specified in the industry standard.

Key words: metal corrosion, Ce (Ⅳ) decontamination, ultrasonic decontamination

中图分类号:

TL944

杨蕊, 曲啸虎, 郑开元, 田春平, 郭晋汉, 王钊, 刘婷婷, 周羽, 高杨. 用于压水堆一回路去污的Ce（Ⅳ）+超声去污技术研究[J]. 辐射防护, 2025, 45(S1): 18-25.

YANG Rui, QU Xiaohu, ZHENG Kaiyuan, TIAN Chunping, GUO Jinhan, WANG Zhao, LIU Tingting, ZHOU Yu, GAO Yang. Study on Ce (Ⅳ) plus ultrasonic decontamination technology for primary circuit decontamination of PWR[J]. RADIATION PROTECTION, 2025, 45(S1): 18-25.

参考文献

[1] HU Yanze, LONG Xinggui, DONG Lan, et al.A decontamination technique for the primary cooling circuit of the research type nuclear reactor[J]. Nuclear Engineering and Design, 2018, 337: 318-323.
[2] Rafique M, Mirza N M, Mirza S M.Kinetic study of corrosion product activity in primary coolant pipes of a typical PWR under flow rate transients and linearly increasing corrosion rates[J]. Journal of Nuclear Materials, 2005, 346(2/3): 282-292.
[3] Hirschberg G, Baradlai P, Varga K, et al.Accumulation of radioactive corrosion products on steel surfaces of VVER type nuclear reactors. I. ^110mAg[J]. Journal of Nuclear Materials, 1999, 265(3): 273-284.
[4] 刘斌, 李新民, 宋利君, 等. 压水堆核电站在役化学去污工艺进展[J]. 辐射防护通讯, 2015, 35(2): 16-20.
[5] 王鹏, 夏良树. 核设备在役去污技术现状及发展趋势[J]. 化学工程与装备, 2017(5): 193-195.
[6] 王邵, 刘坤贤, 张天祥.核设施退役工程[M]. 北京: 中国原子能出版社, 2013: 64-133.
[7] Murray A P.A chemical decontamination process for decontaminating and decommissioning nuclear reactors[J]. Nuclear Technology, 1986, 74(3): 324-332.
[8] Suwa T, Kuribayashi N, Tachikawa E.Development of chemical decontamination process with sulfuric acid-cerium (Ⅳ) for decommissioning[J]. Journal of Nuclear Science & Technology, 1988, 25(7): 574-585.
[9] 刘刈, 陈艳, 孔彦荣, 等. 超声波+四价铈去污技术研究[J]. 辐射防护, 2017, 37(1): 39-44.
[10] 仪表功能材料标准化技术委员会. 金属材料实验室均匀腐蚀全浸试验方法: JB/T 7901—1999[S]. 北京: 国家机械工业局, 2010.
[11] Suwa T, Kuribayashi N, Tachikawa E.Development of chemical decontamination process with sulfuric acid-cerium (Ⅳ) for decommissioning[J]. Journal of Nuclear Science & Technology, 1992, 23(7): 622-632.
[12] 肖茜. 反应堆压力容器用低合金钢及不锈钢堆焊层在模拟压水堆一回路水中的腐蚀行为[D]. 上海: 上海大学, 2018.
[13] 林玉珍, 杨德钧. 腐蚀和腐蚀控制原理[M]. 北京: 中国石化出版社, 2007.
[14] 魏鑫, 徐乐昌, 仇月双, 等. 化学与超声协同去除铀放射性污染研究[J]. 原子能科学技术, 2023, 57(S1): 18-25.
[15] 能源行业核电标准化技术委员会. 压水堆核电厂一回路系统及设备化学去污导则: NB/T 20142—2012[S]. 北京: 国家能源局, 2012.