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 |
ISSN | 0003-2700 |
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. |
DOI | 10.1021/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 | |
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 |
推荐引用方式 GB/T 7714 | 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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