通过 spICP-TOFMS 对亚微米颗粒进行同位素比值分析

IF 3.1 2区 化学 Q2 CHEMISTRY, ANALYTICAL
Sarah E. Szakas and Alexander Gundlach-Graham
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引用次数: 0

摘要

我们研究了使用单颗粒电感耦合等离子体飞行时间质谱法(spICP-TOFMS)测量单个亚微米颗粒内的同位素比率,并探讨了这种方法的优势和局限性。通过分析单个独居石颗粒中的硒(Sm)同位素--147Sm 和 149Sm,以及单个方铅矿颗粒中的铅(Pb)同位素--206Pb 和 208Pb,我们证明了 spICP-TOFMS 记录的同位素比的精度受泊松统计的控制。这种精确度取决于从单个颗粒中测量到的每种同位素的信号量:随着颗粒尺寸的增大,每种同位素被检测到的次数增多,精确度也随之提高。在 Sm 质量从 40 ag 到 4 fg 的独居石颗粒中,同位素比率精度(相对标准偏差,RSD)从 43% 到 5% 不等。不过,颗粒群的平均同位素比值仍然是准确的;149Sm/147Sm 的摩尔比值为 0.912,与预期比值相差 1%。由于 206Pb、207Pb 和 208Pb 是由钍(Th)和铀(U)衰变而来的放射性同位素,因此铅的同位素组成在自然界中变化很大。在对方铅矿颗粒中的铅同位素进行分析时,我们发现,对于铅含量为 1.4 fg 至 80 fg 的颗粒,208Pb/206Pb 比率的 RSD 为 32% 至 2%。我们进一步探索了利用 spICP-TOFMS 对独居石颗粒进行辐射测定的方法。对仅含 0.02-80 fg Th 和 0.03-30 fg U 的单个独居石颗粒进行的 spICP-TOFMS 分析显示了放射性铅同位素特征和 550 Ma 的中位年龄。我们还表明,独居石颗粒的年龄分布比泊松统计所能解释的范围更广,揭示了颗粒中年龄或铅、钍和/或铀的贫化/富集的真实变化。总之,我们证明了 spICP-TOFMS 可用于精确的同位素比值分析,精确度可低至百分之几;然而,了解测量噪声对于确定从单个颗粒测得的同位素比值的意义至关重要。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Isotopic ratio analysis of individual sub-micron particles via spICP-TOFMS†

Isotopic ratio analysis of individual sub-micron particles via spICP-TOFMS†

We investigate the use of single particle inductively coupled plasma time-of-flight mass spectrometry (spICP-TOFMS) to measure isotopic ratios within individual sub-micron particles and explore the advantages and limitations of this method. Through the analysis of samarium (Sm) isotopes—147Sm and 149Sm—in individual monazite particles, and lead (Pb) isotopes—206Pb and 208Pb—in individual galena particles, we demonstrate that isotope ratios recorded by spICP-TOFMS have precision controlled by Poisson statistics. This precision depends on the signal amount measured per isotope from an individual particle: as particle size increases, more counts of each isotope are detected, and the precision improves. In monazite particles with mass amounts of Sm from 0.04 to 4 fg, recorded isotope-ratio precision (relative standard deviation, RSD) ranged from 43% to 5%. However, the average isotope ratio from a particle population is still accurate; the molar ratio determined for 149Sm/147Sm was 0.912, which is within 1% of the expected ratio. Lead isotopic composition varies widely in nature because 206Pb, 207Pb, and 208Pb are radiogenic isotopes that decay from thorium (Th) and uranium (U). In the analysis of lead isotopes from galena particles, we found that the RSD for 208Pb/206Pb ratio ranged from 32% to 2% for particles with 1.4 to 80 fg of Pb. We further explore the use of spICP-TOFMS for radiometric dating of monazite particles. Monazite is used in geochronology for radiometric dating based on 208Pb/232Th and 206Pb/238U ratios. spICP-TOFMS analyses of individual monazite particles that contain only 0.02–80 fg of Th and 0.03–30 fg of U showed radiogenic Pb-isotope signatures and a median age of 550 Ma. We also show that the spread of ages from monazite particles is broader than explainable by Poisson statistics, revealing real variation in age or depletion/enrichment of Pb, Th, and/or U in the particles. Overall, we demonstrate that spICP-TOFMS can be used for accurate isotope-ratio analysis with precisions down to a few percent; however, understanding measurement noise is critical to define the significance of isotope ratios measured from individual particles.

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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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