Investigation of direct simultaneous uranium isotopic determination and age dating of micrometer-sized uranium particles by laser ablation – multi-collector ICPMS†

IF 3.1 2区 化学 Q2 CHEMISTRY, ANALYTICAL
Anne-Claire Humbert, Fabien Pointurier and Amélie Hubert
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Abstract

In this study, we demonstrate that it is possible to simultaneously determine accurate uranium 234U and 235U abundances and the date of purification (or “age”) of uranium oxide materials at the particle scale using laser ablation – multi-collector ICPMS coupling. The method was successfully applied to microparticles of uranium materials enriched at 5%, 85% and 90% and purified 70 years ago. The deviations from the reference age are, at most, respectively 6 years, 2 years and 1 month which is comparable to what can be obtained using the reference technique LG-SIMS. The precision of 235U abundances and 234U abundances, at the particle scale, was respectively between 0.11% and 1.95% and between 0.4% and 5% which is equivalent to or better than what was previously published for the analyses of depleted to moderately enriched materials by LA-ICPMS, showing that adding 230Th determination doesn't degrade the determination of 234U and 235U abundances. Due to the small amount of material introduced into the ICPMS, μm-sized particle analysis by LA-ICPMS has the advantage of being less subject to laser-induced fractionation than bulk material analyses by LA-ICPMS. In contrast to the latter, a correction for uranium versus thorium fractionation can be applied based on the measurement of their relative sensitivities in standard solutions.

Abstract Image

通过激光烧蚀-多收集器 ICPMS† 对微米级铀粒子进行直接同步铀同位素测定和年代测定的研究
在本研究中,我们证明了利用激光烧蚀-多收集器 ICPMS 耦合技术,可以同时准确测定铀氧化物材料在颗粒尺度上的铀 234U 和 235U 丰度以及提纯日期(或 "年龄")。该方法成功应用于富集度为 5%、85% 和 90%、纯化时间为 70 年前的铀材料微粒。与参考年龄的偏差最多分别为 6 年、2 年和 1 个月,与使用参考技术 LG-SIMS 所获得的结果相当。在颗粒尺度上,235U 丰度和 234U 丰度的精度分别为 0.11% 至 1.95% 和 0.4% 至 5%,相当于或优于之前发表的用 LA-ICPMS 分析贫化至中度富集材料的结果,这表明加入 230Th 测定并不会降低 234U 和 235U 丰度的测定结果。由于进入 ICPMS 的物质数量较少,用 LA-ICPMS 分析微米大小的颗粒与用 LA-ICPMS 分析块状物质相比,具有受激光诱导分馏影响较小的优势。与后者不同的是,可以根据标准溶液中铀和钍相对灵敏度的测量结果,对铀和钍的分馏进行校正。
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来源期刊
CiteScore
6.20
自引率
26.50%
发文量
228
审稿时长
1.7 months
期刊介绍: Innovative research on the fundamental theory and application of spectrometric techniques.
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