Rapid isotopic analysis of uranium microparticles via SP-ICP-TOF-MS

IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Jordan S. Stanberry , Sarah E. Szakas , Hunter B. Andrews , Lyndsey Hendriks , Brian W. Ticknor , Rachel A. Bergin , Shawna K. Tazik , Philip Kegler , Stefan Neumeier , N. Alex Zirakparvar , Daniel R. Dunlap , Benjamin T. Manard
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Abstract

Inductively coupled plasma – time-of-flight – mass spectrometry (ICP-TOF-MS) was employed for the isotopic analysis of uranium particles of varying 235U enrichment levels. Here, a single particle (SP)-based introduction scheme was employed such that individual particles, in a suspension, were analyzed. The uranium oxide microparticles were comprised of depleted uranium (DU, 235U/238U of 0.0017316(14)), natural uranium (NU, 235U/238U of 0.0072614(39)), and low enriched uranium (LEU, 235U/238U of 0.051025(15)). The percent relative difference of the SP-ICP-TOF-MS measured isotopic ratios compared to the expected values for the DU, NU, and LEU particle populations were 8.75, 0.12, and 1.23 %, respectively. After characterization, the DU and NU particles were doped within a complex sample matrix (Arizona Test Dust) containing Fe, Ti, Al, and Si particles, among others. Then, the suspension was analyzed via SP-ICP-TOF-MS and the detected particles were classified as DU or NU based on their measured 235U/238U ratio. In the same analysis, the matrix particles (i.e., Al, Fe, and Ti) were detected, demonstrating the simultaneous nuclide detection provided by the measurement platform. The presented SP-ICP-TOF-MS methodology for uranium particle characterization proved to be a high throughput method for detecting and isotopically discerning uranium particles with varying enrichment levels, in a complex matrix.

Abstract Image

SP-ICP-TOF-MS快速分析铀微粒同位素
采用电感耦合等离子体-飞行时间-质谱法(ICP-TOF-MS)对不同铀浓缩水平的铀粒子进行了同位素分析。在这里,采用基于单粒子(SP)的引入方案,以便对悬浮液中的单个粒子进行分析。氧化铀微粒由贫铀(DU, 235U/238U为0.0017316(14))、天然铀(NU, 235U/238U为0.0072614(39))和低浓缩铀(LEU, 235U/238U为0.051025(15))组成。SP-ICP-TOF-MS测量的同位素比率与DU、NU和LEU粒子群期望值的相对差异百分比分别为8.75%、0.12%和1.23%。表征后,将DU和NU颗粒掺杂在含有Fe, Ti, Al和Si颗粒等的复杂样品基质(Arizona Test Dust)中。然后,通过SP-ICP-TOF-MS对悬浮液进行分析,并根据其测量的235U/238U比值将检测到的颗粒分类为DU或NU。在同一分析中,检测到基体颗粒(即Al, Fe和Ti),证明了测量平台提供的同时检测核素。本文提出的SP-ICP-TOF-MS方法是一种高通量的方法,用于在复杂基质中检测和同位素识别不同富集水平的铀颗粒。
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来源期刊
Talanta
Talanta 化学-分析化学
CiteScore
12.30
自引率
4.90%
发文量
861
审稿时长
29 days
期刊介绍: Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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