Extractive Electrospray Ionization Mass Spectrometry for Sensitive Detection of Uranyl Species in Natural Water Samples

Extractive Electrospray Ionization Mass Spectrometry for Sensitive Detection of Uranyl Species in Natural Water Samples
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DOI:
10.1021/ac9019494
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发表时间:
2010-01-01
影响因子:
7.4
通讯作者:
Huan, Yanfu
Huan, Yanfu
中科院分区:
化学1区
文献类型:
--
作者:
Luo, Mingbiao;Hu, Bin;Huan, Yanfu

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环境质谱法越来越多地应用于复杂基质中痕量有机化合物的灵敏检测。在现实世界中,检测痕量无机物种,特别是具有物种形成信息的无机物种具有重要意义。建立了一种萃取电喷雾电离串联质谱(MS/MS)快速检测天然水样中放射性无机物质的方法。带负电荷的醋酸铀酰在气相中经历了特有的破碎,为复杂基质中铀酰物种的特异性检测提供了基础化学,而无需样品预处理。在优化的实验条件下,采用多级EESI质谱法对不同天然水样中的铀酰进行了快速检测。每次样品分析的平均时间约为10 s。利用EESI-MS3实验获得的特征碎片,铀的检出限约为10(-3)ng/L。8次测量的典型相对标准偏差(RSD)为6.9,与8.1%相近(S/N = 3)。动态响应范围为10(-1),与水样中铀的10(3)ng/L相似。采用EESI-MS实验定量检测铀酰物种的同位素比值。结果表明,EESI-MS作为一种典型的有机化合物分析方法,在实时在线监测天然水样中铀酰等无机物质方面具有广阔的应用前景。
Ambient mass spectrometry has been increasingly applied for sensitive detection of trace organic compounds present in complex matrixes. In the real world, detection of trace amounts of inorganic species, particularly with speciation information, is of great significances. Herein a method based on extractive electrospray ionization (EESI) tandem mass spectrometry (MS/MS) has been established for rapid detection of radioactive inorganic species in natural water samples. Negatively charged uranyl acetate undergoes characteristic fragmentation in the gas phase, providing the fundamental chemistry for specific detection of uranyl species in complex matrixes without sample pretreatment. Under the optimized experimental conditions, uranyl species in various natural water samples were rapidly detected using multiple-stage EESI mass spectrometry. The mean time for each sample analysis was about 10 s. The limit of detection was about a few 10(-3) ng/L of uranium by utilizing the characteristic fragments obtained in the EESI-MS3 experiments. The typical relative standard deviation (RSD) of this method was 6.9 similar to 8.1% for 8 measurements (S/N = 3). The dynamic response range was 10(-1)similar to 10(3) ng/L for uranium in water samples. The isotope ratio of uranyl species was quantitatively detected using EESI-MS experiments. The results show that EESI-MS, a typical method initially developed for organic compound analysis, has promising perspectives for real time, online monitoring of inorganic species such as uranyl species in natural water samples.