Isotopic analysis of uranium and plutonium using ICP-MS and estimation of burn-up of spent uranium in contaminated environmental samples
Isotopic analysis of uranium and plutonium using ICP-MS and estimation of burn-up of spent uranium in contaminated environmental samples
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DOI：
10.1039/b202196j
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发表时间：
2002-01-01
影响因子：
3.4
通讯作者：
Becker, JS
中科院分区：
文献类型：
--
作者：
Boulyga, SF;Becker, JS
放射性元素环境监测和污染源评估(核武器试验、核电厂和核后处理厂事故等)需要精确和准确的氡系元素的同位素分析，特别是铀和钚。采用双聚焦扇场电感耦合等离子体质谱(ICPSFMS)，采用带膜去溶的低流量微同心雾化器“ARIDUS”，在超痕量水平上测量铀和钚的同位素。化学萃取后U-236和Pu-239在水溶液和土壤中的检出限分别为0.2pg·L(-1)和0.04pg·g(-1)。测定了切尔诺贝利核电站周围30公里范围内土壤样品中U-235/U-238、U-236/U-238和Pu-240/Pu-239的同位素比值。污染表层土壤中Pu-240/Pu-239的平均同位素比值为0.396+/-0.014。用迭代法计算了土壤中废铀/天然铀混合物的燃耗等级和废铀所占比例。通过对U-235/U-238和U-236/U-238同位素比值的分析，发现乏反应堆铀的燃耗等级略有变化。观察到Pu-240/Pu-239同位素比值与乏铀燃耗之间的关系。
Environmental monitoring of actinides and evaluation of the contamination source (nuclear weapons tests, nuclear power plant and nuclear reprocessing plant accidents, etc.) requires precise and accurate isotopic analysis of actinides, especially uranium and plutonium. Double-focusing sector-field inductively coupled plasma mass spectrometry (ICP-SFMS) using a low-flow microconcentric nebulizer with membrane desolvation, "Aridus'', was applied for isotopic measurements of uranium and plutonium at the ultratrace level. The detection limit (3sigma) for U-236 and Pu-239 after chemical extraction was 0.2 pg l(-1) in aqueous solution and 0.04 pg g(-1) in soil, respectively. U-235/U-238, U-236/U-238 and Pu-240/Pu-239 isotope ratios were measured in soil samples collected within the 30 km zone around the Chernobyl nuclear power plant. The average Pu-240/Pu-239 isotope ratio in contaminated surface soil was 0.396+/-0.014. The burn-up grade and the portion of spent uranium in the spent uranium/natural uranium mixture in soil were calculated using the iteration method. A slight variation in the burn-up grade of spent reactor uranium was revealed by analyzing U-235/U-238 and U-236/U-238 isotope ratios. A relationship between the Pu-240/Pu-239 isotope ratio and burn-up of spent uranium was observed.