水热法合成铯榴石及其在含铯废水处理中的应用研究

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摘要： 通过模拟自然界中沸石分子筛的形成条件,利用水热法合成铯榴石处理含铯废液,在此基础上,设计正交试验,对合成工艺参数进行了优化及验证,并对合成的铯榴石进行了抗浸出性、耐辐照性测试。结果表明:利用水热法合成铯榴石处理含铯废水的方法可有效去除废水中的铯,最优合成工艺条件为:溶胶的组成为:1.0 SiO₂∶0.35 Al₂O₃∶0.95 Na₂O∶84 H₂O,温度为171 ℃,反应时长为48 h,在此条件下对废水中铯的去除率可达99%以上;经测试合成的铯榴石具有较强的抗浸出性、耐辐照性,可作为放射性铯离子的处置材料。

关键词: 铯榴石, 水热法, 除铯, 工艺验证

Abstract: Cesium is easily soluble in water, and has a good migration rate and a low boiling point, making it difficult to dispose of safely. The safe disposal of radioactive cesium is an urgent problem to be solved. Current technologies used for cement fixation and solidification, and ion exchange have certain shortcomings in the treatment of cesium containing waste liquid, and further optimization is urgently needed. Pollucite belongs to the zeolite type molecular sieve, with a suitable pore size. Without damaging the structure of pollucite, radioactive cesium cannot diffuse out of it. Many studies have shown that it is one of the potential ultimate choices for disposing of radioactive cesium. In previous studies, pollucite needs to be synthesized at high temperatures above 1 000 ℃, which can cause the volatilization of cesium and increase the difficulty of tail gas treatment. This study used hydrothermal method to simulate the generation environment of molecular sieve zeolites in nature and achieved the synthesis of pollucite at lower temperatures. Through a 2 L/batch treatment device, the cesium containing waste liquid is treated, with a removal rate of over 99% for cesium in the wastewater. This study also tested the leaching resistance, thermal stability, and radiation resistance of cesium, confirming its strong stability and suitability as a radioactive disposal material.

Key words: pollucite, hydrothermal method, cesium removal, process validation

中图分类号:

TL941+.1

于伟跃, 高凯, 王浩, 谭俊, 杨彪, 林海鹏. 水热法合成铯榴石及其在含铯废水处理中的应用研究[J]. 辐射防护, 2025, 45(2): 175-181.

YU Weiyue, GAO Kai, WANG Hao, TAN Jun, YANG Biao, LIN Haipeng. Research on hydrothermal method for stable treatment of free cesium in wastewater[J]. RADIATION PROTECTION, 2025, 45(2): 175-181.

[1] 罗静, 钟辉, 徐粉燕. 从高放废液中分离铯的研究进展[J]. 广东微量元素科学, 2007, 14(10): 6-10.
LUO Jing, ZHONG Hui, XU Fenyan. Research progress of separation of Cs from high-level radioactive liquid waste[J]. Guangdong Trace Elements Science, 2007, 14(10): 6-10.
[2] 姜长印, 王士柱, 宋崇立, 等. 用亚铁氰化钾钛从高放废液中去除铯的研究[J]. 核化学与放射化学, 1995(2): 99-104.
[3] 于波, 陈靖, 朱晓文, 等. 从酸性高放废液中去除¹³⁷Cs的研究进展[J]. 原子能科学技术, 2002(1): 51-57.
[4] Hassan N M. Adsorption of Cesium from spent nuclear fuel basin water[J]. Journal of Radioanalytical and Nuclear Chemistry, 2005, 266(1): 57-59.
[5] 陈良, 陈莉, 李均华. 压水堆核电站放射性废液水泥固化技术分析[J]. 核动力工程, 2009, 30(2): 113-116+123.
CHEN Liang, CHEN Li, LI Junhua. Aanalysis of cementation technology for liquid radioactive-waste in PWR NPPs[J]. Nuclear Power Engineering, 2009, 30(2): 113-116+123.
[6] Abdel Rahman R O,Zin El Abidin D H A, Abou-Shady H. Cesium binding and leaching from single and binary contaminant cement-bentonite matrices[J]. Chemical Engineering Journal, 2014, 245: 276-287.
[7] 谷万成. 低中水平放射性废液的水泥固化研究[J]. 湿法冶金, 2005, 24(1): 33-39.
GU Wancheng. Cement solidification of low and intermediate level radioactive effluent[J]. Hydrometallurgy of China, 2005, 24(1): 33-39.
[8] 高亚. 模拟高盐高碱中低水平放射性废液水泥固化技术研究[D]. 绵阳: 西南科技大学, 2014.
[9] Plecas I, Peric A, Kostadinovic A, et al. Leaching behavior of ⁶⁰Co and ¹⁷³Cs from spent ion exchange resins in cement matrix[J]. Cement & Concrete Research, 1992, 22(5): 937-940.
[10] Abusafa A, Yücel H. Removal of ¹³⁷Cs from aqueous solutions using different cationic forms of a natural zeolite: clinoptilolite[J]. Separation and Purification Technology, 2002, 28(2): 103-116.
[11] 刘爱平, 刘岁海, 汪惠. 斜发沸石处理模拟含铯放射性废水研究[J]. 金属矿山, 2012(4): 148-151.
LIU Aiping, LIU Suihai, WANG Hui. Treatment of simulated radioactive waste water containing Cs⁺ with clinoptilotite[J]. Metal Mine, 2012(4): 148-151.
[12] GU B X, WANG L M, Ewing R C. The effect of amorphization on the Cs ion exchange and retention capacity of zeolite-NaY[J]. Journal of Nuclear Materials, 2000, 278(1): 64-72.
[13] Dyer A, Mikhail K Y. The use of zeolites for the treatment of radioactive waste[J]. Mineralogical Magazine, 1985, 49(351): 203-210.
[14] LUO Min, WEN Mingfen, WANG Jianchen, et al. The study of cooperation solidification of Cs based on ZSM-5 zeolite[J]. Energy Procedia, 2013, 39: 434-442.
[15] LI Jun, DUAN Jianxia, HOU Li, et al. Effect of Cs content on K_1-xCs_xAlSi₂O₆ ceramic solidification forms[J]. Journal of Nuclear Materials, 2018, 499: 144-154.
[16] Omerašević M, Ljiljana M, Jovana R, et al. Safe trapping of Cesium into pollucite structure by hot-pressing method[J]. Journal of Nuclear Materials, 2016, 474: 35-44.
[17] HE Peigang, WANG Ruifei, FU Shuai, et al. Safe trapping of Cesium into doping-enhanced pollucite structure by geopolymer precursor technique[J]. Journal of Hazardous Materials, 2019, 367: 577-588.
[18] Duy Quang N, Eba H, Sakurai K. Versatile chemical handling to confine radioactive Cesium as stable inorganic crystal[J]. Scientific Reports, 2018, 8(1): 15051.
[19] Yanagisawa K, Nishioka M, Yamasaki N, et al. Immobilization of Cesium into pollucite structure by hydrothermal hot-pressing[J]. Journal of Nuclear Science and Technology, 1987, 24(1): 51-60.
[20] Yokomori Y, Asazuki K, Kamiya N, et al. Final storage of radioactive Cesium by pollucite hydrothermal synthesis[J]. Scientific Reports, 2014, 4: 4195.
[21] 高凯, 冯文东, 薛海龙, 等. 一种放射性含铯废水的处理方法: CN113436772B[P]. 2022-07-29.
[22] 李军, 侯莉, 卢忠远. 钾/钠离子对水热合成铯榴石结构的影响[J]. 原子能科学技术, 2019, 53(1): 50-58.
LI Jun, HOU Li, LU Zhongyuan. Eeffect of K⁺/Na⁺ on structure of hydrothermal synthesized pollucite[J]. Atomic Energy Science and Technology, 2019, 53(1): 50-58.
[23] 江苏省环境监测中心, 苏州市环境监测中心站. 水质 65种元素的测定电感耦合等离子体质谱法: HJ 700—2014[S]. 北京: 中国环境科学出版社出版, 2014.
[24] Jantzen C M, Bibler N E. The product consistency test (ASTM C1285-02) for waste form durability testing[M]// Environmental Issues and Waste Management Technologies in the Ceramic and Nuclear Industries XI. New York: Wiley, 2006: 141-151.
[25] 王大伟. 硼硅酸盐玻璃浸出行为的研究[D]. 兰州: 兰州大学, 2012.
[26] Malkovsky V I, Yudintsev S V, Ojovan M I, et al. The influence of radiation on confinement properties of nuclear waste glasses[J]. Science and Technology of Nuclear Installations, 2020, 8875723: 14.

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