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水样中237Np、239~241Pu和241Am快速同时分析OA

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

中文摘要英文摘要

核应急状况下需要对放射性污染的水平和程度进行快速评估,其中高毒性超铀核素(237Np、239~241Pu和241Am)的快速同时分析尤为重要.然而针对同一样品中多种难分析放射性核素的测定,目前报道的方法需要使用多种色谱分离树脂对其分别进行分离,操作流程繁琐耗时,难以满足快速响应的需求.本工作将基于DGA树脂的核素色谱分离与三重四极杆电感耦合等离子体质谱(ICP-MS/MS)测量技术相结合,建立了一种能够同时测定水样中多种超铀核素的快速分析方法.该方法分别使用242Pu和243Am作为Np/Pu和Am的示踪剂,化学产率均大于80%.使用ICP-MS/MS的He-O2模式,基于237Np、239~241Pu和241 Am与O2的反应速率不同,实现了同一待测液中所有目标核素浓度的直接同时测量.实验表明,在8.0 mL/min He-0.37 mL/min O2条件下,241Pu和241 Am的交叉污染小于1%.方法对这些超铀核素的检测限达到fg量级,每批样品的分析时间小于2.5 h,满足核应急分析需求.使用标准加入法对建立的分析方法进行了验证,结果表明其准确可靠.

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.

彭晨阳;王浩;张峰;邢闪;史克亮;侯小琳

兰州大学核科学与技术学院,甘肃兰州 730000兰州大学核科学与技术学院,甘肃兰州 730000兰州大学核科学与技术学院,甘肃兰州 730000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

能源科技

ICP-MS/MSHe-O2模式色谱分离超铀核素

ICP-MS/MSHe-O2 modechromatographic separationtransuranium nuclide

《原子能科学技术》 2026 (4)

848-857,10

国家自然科学基金(U21A20442,22341603)

10.7538/yzk.2025.youxian.0521

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