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Determination of Femtogram-Level Plutonium Isotopes in Environmental and Forensic Samples with High-Level Uranium Using Chemical Separation and ICP-MS/MS Measurement
Hou, Xiaolin1,2,3,5; Zhang, Weichao1,4; Wang, Yanyun1,4
通讯作者Hou, Xiaolin(xiho@dtu.dk)
2019-09-17
发表期刊ANALYTICAL CHEMISTRY
ISSN0003-2700
卷号91期号:18页码:11553-11561
摘要ICP-MS is becoming a competitive technique for measurement of plutonium isotopes. Besides the abundance sensitivity (tailing of U-238 to m/z = 239 and 240), isobaric and polyatomic ions interferences (e.g., (UH+)-U-238-H-1) are the most critical challenges for determination of low-level plutonium in high uranium samples. This work presents a new method to solve this problem using ICP-MS with two tandem quadrupole separators and a dynamic collision/reaction cell combined with chemical separation. The interference of uranium hydrides ((UH+)-U-238-H-1 and (UH2+)-U-238-H-1) was effectively eliminated using CO2 as reaction gas by converting hydrides to oxides of uranium ions (UO+/UO2+) but still keeping the intensity of the Pu+ signal. The tailing interference of U-238(+) (abundance sensitivity) was intensively eliminated by significantly suppressing the U-238(+) signal using CO2 as reaction gas and using two tandem quadrupole mass separators in the ICP-MS/MS. With these approaches the overall interference of uranium was reduced to <1 x 10(-8), which is 3 orders of magnitude better than the conventional ICP-MS. Combined with chemical separation with a decontamination factor of 10(5) for uranium, an overall factor of 10(12) for elimination of uranium interference was achieved. The developed method was demonstrated to enable accurate determination of <10(-15) g/g level plutonium isotopes in environmental samples even in a uranium debris sample with a U/Pu atomic ratio of up to 10(12). The developed method was validated by analysis of a spiked solution and certified reference materials of soil.
DOI10.1021/acs.analchem.9b01347
关键词[WOS]PLASMA-MASS SPECTROMETRY ; ULTRA-TRACE DETERMINATION ; PU ISOTOPES ; REACTION CELL ; GLOBAL FALLOUT ; ATOM RATIOS ; PU-240 ; SOIL ; RESOLUTION ; MS
收录类别SCI ; SCI
语种英语
资助项目National Natural Science Foundation of China[11605206] ; National Natural Science Foundation of China[11875261] ; National Natural Science Foundation of China[41603125] ; National Natural Science Foundation of China[91643206] ; Ministry of Science and Technology of China[2015FY110800] ; Chinese Academy of Sciences[132B61KYSB20180003] ; National Research Program for Key Issues in Air Pollution Control[DQGG0105-02]
WOS研究方向Chemistry
项目资助者National Natural Science Foundation of China ; Ministry of Science and Technology of China ; Chinese Academy of Sciences ; National Research Program for Key Issues in Air Pollution Control
WOS类目Chemistry, Analytical
WOS记录号WOS:000487156900012
出版者AMER CHEMICAL SOC
引用统计
被引频次:37[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ieecas.cn/handle/361006/13358
专题加速器质谱中心
第四纪科学与全球变化卓越创新中心
通讯作者Hou, Xiaolin
作者单位1.Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol,Xian AMS Ct, Shaanxi Key Lab Accelerator Mass Spectrometry Tec, Xian 710061, Shaanxi, Peoples R China
2.Tech Univ Denmark, DTU Nutech, Ctr Nucl Technol, DK-4000 Roskilde, Denmark
3.CAS Ctr Excellence Quaternary Sci & Global Change, Xian 710061, Shaanxi, Peoples R China
4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
5.Pilot Natl Lab Marine Sci & Technol Qingdao, Open Studio Ocean Continental Climate & Environm, Qingdao 266061, Shandong, Peoples R China
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Hou, Xiaolin,Zhang, Weichao,Wang, Yanyun. Determination of Femtogram-Level Plutonium Isotopes in Environmental and Forensic Samples with High-Level Uranium Using Chemical Separation and ICP-MS/MS Measurement[J]. ANALYTICAL CHEMISTRY,2019,91(18):11553-11561.
APA Hou, Xiaolin,Zhang, Weichao,&Wang, Yanyun.(2019).Determination of Femtogram-Level Plutonium Isotopes in Environmental and Forensic Samples with High-Level Uranium Using Chemical Separation and ICP-MS/MS Measurement.ANALYTICAL CHEMISTRY,91(18),11553-11561.
MLA Hou, Xiaolin,et al."Determination of Femtogram-Level Plutonium Isotopes in Environmental and Forensic Samples with High-Level Uranium Using Chemical Separation and ICP-MS/MS Measurement".ANALYTICAL CHEMISTRY 91.18(2019):11553-11561.
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