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水样中237Np、239~241Pu和241Am快速同时分析

彭晨阳 王浩 张峰 邢闪 史克亮 侯小琳

原子能科学技术2026,Vol.60Issue(4):848-857,10.
原子能科学技术2026,Vol.60Issue(4):848-857,10.DOI:10.7538/yzk.2025.youxian.0521

水样中237Np、239~241Pu和241Am快速同时分析

Rapid Simultaneous Determination of 237Np,239-241Pu and 241Am in Water Samples

彭晨阳 1王浩 1张峰 1邢闪 2史克亮 2侯小琳2

作者信息

  • 1. 兰州大学核科学与技术学院,甘肃兰州 730000
  • 2. 兰州大学核科学与技术学院,甘肃兰州 730000||兰州大学核生化灾害防护化学全国重点实验室,甘肃兰州 730000||兰州大学稀有同位素前沿科学中心,甘肃兰州 730000
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摘要

Abstract

In nuclear emergency,it is crucial to quick assess the level and extent of radioactive contamination.Highly toxic transuranic nuclides(237Np,239-241Pu and 241Am)are the most important radionuclides in radioactive contamination.In the case for analysis of multiple radionuclides in the same sample,the reported analytical methods are often time-consuming/tedious by using multiple chromatographic separation resins for the separation of every single radionuclide.In this work,a rapid analytical method for simultaneously determining transuranium nuclides in water samples was developed by coupling triple quadrupole inductively coupled plasma mass spectrometry(ICP-MS/MS)with a single DGA resin column,Np,Pu,and Am were simultaneously enriched and purified.For monitoring chemical yields of Np/Pu and Am,the chemical recoveries are greater than 80%which is monitored using 242Pu and 243Am as tracers.O2 was used as reaction gas in the collision reaction cell(CRC)of ICP-MS/MS,the chemical reaction behavior of Np and Pu with O2 is similar,and Np/Pu reacts with O2 and converts to NpO2+/PuO2,and Am reacts with O2 and concerts to AmO+.237Np,239-241Pu and241 Am in the same solution were simultaneously measured by the He-O2 mode of ICP-MS/MS in the same run,and the cross contamination of 241Pu and 241Am(<1%)was achieved using 8.0 mL/min He-0.37 mL/min O2 as reaction gas.A sensitivity of 814×106 s-1/(mg/L)for Np,799× 106 s-1/(mg/L)for Pu,and 1 027× 106 s-1/(mg/L)for Am is achieved,and the sensitivity ratio of NpO2+and PuO2+is close to 1,indicating that 242Pu is feasible as a non-isotope tracer of Np under this condition.The abundance sensitivity of U and the interference of polyatomic ions(1H238U+,1H2238U+,206Pb35Cl+,204Pb37Cl+,204Hg37Cl+,205Tl36Ar+and 209Bi16O2+)formed by U and matrix elements(Pb,Hg,Tl and Bi)are effectively inhibited.The detection limit(DL)of 1.84 fg/L for 237Np,2.08 fg/L for 239Pu,0.70 fg/L for 240Pu,0.66 fg/L for 241Pu and 1.27 fg/L for241 Am are approached,this is three orders of magnitude lower than the DL required in nuclear emergency situations(1 Bq/L).The developed method is validated by analyzing the spiked samples,and allows for the rapid,simultaneous detection of ultra-trace amounts of Np,Pu and Am in environmental water samples within 2.5 h.This significantly reduces analysis time and meets the requirement for emergency preparedness.

关键词

ICP-MS/MS/He-O2模式/色谱分离/超铀核素

Key words

ICP-MS/MS/He-O2 mode/chromatographic separation/transuranium nuclide

分类

能源科技

引用本文复制引用

彭晨阳,王浩,张峰,邢闪,史克亮,侯小琳..水样中237Np、239~241Pu和241Am快速同时分析[J].原子能科学技术,2026,60(4):848-857,10.

基金项目

国家自然科学基金(U21A20442,22341603) (U21A20442,22341603)

原子能科学技术

1000-6931

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