后处理厂气态流出物中I-129的光氧化气溶胶转化方法

摘要/Abstract

摘要： I-129是乏燃料后处理厂气态流出物中典型排放核素,对环境及人体均会产生一定的辐射危害,目前国内暂时缺少针对乏燃料后处理厂气态流出物中I-129的在线监测方法。基于已有的气溶胶在线监测系统,设计气溶胶转化装置,解决气溶胶在线监测系统进样问题,为后续后处理厂气态流出物中气态I-129的在线监测提供进样前处理装置与方法。通过稳定碘代替I-129进行气溶胶转化验证实验,测得不同条件下装置转化效率,并结合ICP-MS性能参数、气溶胶转化装置转化效率及在线监测过程中的气溶胶损失率,初步得出该气溶胶转化装置用于气态流出物中I-129在线监测的探测下限范围,最优气溶胶转化效率可达43.35%,平均相对偏差为5.33%。与国际连续监测探测下限要求进行比对,验证了方法的可行性以及在后处理气态流出物中I-129在线监测领域的较好前景和研究价值。

关键词: 在线监测, 乏燃料后处理, 气态流出物, I-129, 气溶胶转化, ICP-MS

Abstract: I-129 is a typical emission nuclide in the gaseous effluent of spent fuel reprocessing, which will produce certain radiation hazards to the environment and human body. Therefore I-129 needs to be monitored. Until now online monitoring of I-129 in the gaseous effluent of spent fuel reprocessing plant is still vacant in China. Based on the existing aerosol online monitoring system, this paper designs an aerosol conversion device to solve the sampling problem of the aerosol online monitoring system, and provides a pre-sampling device and method for the online monitoring of gaseous I-129 in the gaseous effluent of the reprocessing plant by the subsequent linkage aerosol online monitoring technology. The aerosol conversion experiment was carried out by stable iodine instead of I-129, and the conversion efficiency of the device was measured under different conditions. Combined with the performance parameters of ICP-MS, the conversion efficiency of the aerosol conversion device and the loss rate of aerosol during the online monitoring process, the low detection limit range of the aerosol conversion device for the online monitoring of I-129 in gaseous effluent was preliminarily derived, which was compared with that of the international continuous monitoring low detection limit requirements. The preliminary low detection limit range of the aerosol conversion device for online monitoring of I-129 in gaseous effluent was compared with the international continuous monitoring low detection limit requirements, which verified the feasibility of the method and the better prospect and research value in the field of online monitoring of I-129 in reprocessed gaseous effluent.

Key words: on-line monitoring, spent fuel reprocessing, gaseous effluent, I-129, aerosol conversion, ICP-MS

中图分类号:

TL75+1

蔺一博, 骆志平, 汪传高, 陈然. 后处理厂气态流出物中I-129的光氧化气溶胶转化方法[J]. 辐射防护, 2025, 45(6): 586-594.

LIN Yibo, LUO Zhiping, WANG Chuangao, CHEN Ran. Photo-oxidation aerosol conversion of I-129 in gaseous effluent from reprocessing plants[J]. RADIATION PROTECTION, 2025, 45(6): 586-594.

参考文献

[1] 米宇豪, 以恒冠, 廖运璇, 等. 后处理设施气载流出物中¹²⁹I的监测和监管[J]. 核科学与工程, 2022, 42(1): 207-214.
[2] Kim J, Kim J Y, Bae S E, et al. Review of the development in determination of ¹²⁹I amount and the isotope ratio of ¹²⁹I/¹²⁷I using mass spectrometric measurements[J]. Microchemical Journal, 2021, 169: 106476.
[3] 汪传高, 殷敏, 郑国文, 等. 在线进样ICP-MS用于²³⁹Pu气溶胶活度浓度连续监测技术研究[J]. 原子能科学技术, 2021, 55(12): 2359-2367.
WANG Chuangao, YIN Min, ZHENG Guowen, et al. Continuous ²³⁹Pu aerosol activity concentration monitoring technology based on directed sampling method of ICP-MS[J]. Atomic Energy Science and Technology, 2021, 55(12): 2359-2367.
[4] Henrich E, Huefner R, Sahm A. Improved procedures for efficient iodine removal from fuel solutions in reprocessing plants[J]. Management of Gaseous Wastes From Nuclear Facilities, 1980, K19810265: 139-156.
[5] Auchapt P, Patarin L, Tarnero M. Meeting on fuel reprocessing and waste management,American nuclear society[C]. La Grange Park, IL, USA: American Society for Materials, 1984: 2-3.
[6] Leudet A, Miquel P, Goumondy P J, et al. Balance and behavior of gaseous radionuclides released during initial PWR fuel reprocessing operations[C]//17 DOE nuclear air cleaning conference. Denver, CO (USA): DOE, 1982: 39-181.
[7] Herrmann F J, Motoi V, Herrmann B, et al. Minimizing of iodine-129 release at the Karlsruhe reporcessing plant WAK[C]//22nd Nuclear Air Cleaning and Treatment Conf. Denver: Laboratorium für Aerosolphysik und Filtertechnik, 1992: 230032647.
[8] Weinlaender W, Huppert K L, Weishaupt M. Twenty years of WAK reprocessing pilot plant operation[J]. Proceedings. RECOD ’91, 1991, 1: 55-63.
[9] 韦娜娜, 胡长进, 周闪闪, 等. 大气碘化学与含碘气溶胶形成机制的研究进展[J]. 大气与环境光学学报, 2018, 13(1): 1-19.
[10] LI Yuanxia, ZHAO Jie, DING Yayun, et al. A practical approach of measuring ²³⁸U and ²³²Th in liquid scintillator to sub-ppq level using ICP-MS[J]. Radiation Physics and Chemistry, 2025, 230: 112579.
[11] Wrenn M E, Sohngen J E. Specification and performance of on-site instrumentation for continuously monitoring radioactivity in effluents: IEEE N42.18[S]. New York: Institute of Electrical and Electronics Engineers, 2004.

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