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采用化学分离和 ICP-MS/MS 测定核退役废物样品中的 Cs 浓度和 Cs/Cs 比。

Determination of Cs concentration and Cs/Cs ratio in waste samples from nuclear decommissioning by chemical separation and ICP-MS/MS.

机构信息

Technical University of Denmark, Department of Environmental Engineering, Risø Campus, Roskilde, DK, 4000, Denmark.

Technical University of Denmark, Department of Environmental Engineering, Risø Campus, Roskilde, DK, 4000, Denmark.

出版信息

Talanta. 2021 Jan 1;221:121637. doi: 10.1016/j.talanta.2020.121637. Epub 2020 Sep 8.

DOI:10.1016/j.talanta.2020.121637
PMID:33076157
Abstract

Determination of Cs concentration and Cs/Cs atomic ratio is of great importance in characterization of radioactive waste from decommissioning of nuclear facilities. In this work, an effective analytical method was developed for simultaneously determination of Cs and Cs in different types of waste samples (steel, zirconium alloy, reactor coolant, ion exchange filter paper and spent ion exchange resin) by coupling AMP-PAN, AG MP-1M and AG 50 W-X8 chromatographic separation with ICP-MS/MS measurement. Decontamination factors of 7.0 × 10 for Co, 6.0 × 10 for Ba, 4.2 × 10 for Mo, 3.2 × 10 for Sn and 2.1 × 10 for Sb were achieved using the chemical separation procedure. The overall chemical yields of cesium were higher than 85%. A detection limit of 3.1 × 10 g/g for Cs was achieved for 0.2 g stainless steel sample or spent resin. The developed method was validated by analysis of standard reference materials (IAEA-375) and successfully applied for analysis of zirconium alloy, steel, ion exchange filter paper and spent ion exchange resin from nuclear power reactors. The obtained Cs can be used to evaluate the long-term environmental impact and provide useful information for waste disposal. The measured Cs/Cs ratio in reactor coolant, as a characteristic information, might be useful for source identification and localization of leaked fuel element. The neutron flux of the leaked fuel element can be estimated based on the measured Cs/Cs atomic ratios in the reactor coolant water. The developed method is simple and rapid (8 samples/day) for the determination of Cs concentrations and Cs/Cs ratios in various waste samples from nuclear decommissioning.

摘要

确定 Cs 浓度和 Cs/Cs 原子比对于核设施退役放射性废物的特性描述非常重要。在这项工作中,通过耦合 AMP-PAN、AG MP-1M 和 AG 50 W-X8 色谱分离与 ICP-MS/MS 测量,开发了一种有效分析方法,用于同时测定不同类型废物样品(钢、锆合金、反应堆冷却剂、离子交换滤纸和废离子交换树脂)中的 Cs 和 Cs。采用化学分离程序,Co 的去污因子为 7.0×10,Ba 的去污因子为 6.0×10,Mo 的去污因子为 4.2×10,Sn 的去污因子为 3.2×10,Sb 的去污因子为 2.1×10。Cs 的总化学收率高于 85%。对于 0.2g 不锈钢样品或废树脂,Cs 的检测限达到 3.1×10 g/g。通过对标准参考物质(IAEA-375)的分析验证了所开发方法的有效性,并成功应用于核动力反应堆中锆合金、钢、离子交换滤纸和废离子交换树脂的分析。获得的 Cs 可用于评估长期环境影响,并为废物处置提供有用信息。作为特征信息,反应堆冷却剂中测量的 Cs/Cs 比值可用于泄漏燃料元件的源识别和定位。可根据反应堆冷却水中测量的 Cs/Cs 原子比来估计泄漏燃料元件的中子通量。该方法简单快速(每天 8 个样品),可用于测定核退役过程中各种废物样品中的 Cs 浓度和 Cs/Cs 比值。

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