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一种用于测量小空气样本中羰基硫硫同位素比值的气相色谱-同位素比值质谱法。

A GC-IRMS method for measuring sulfur isotope ratios of carbonyl sulfide from small air samples.

作者信息

Baartman Sophie L, Krol Maarten C, Röckmann Thomas, Hattori Shohei, Kamezaki Kazuki, Yoshida Naohiro, Popa Maria Elena

机构信息

Institute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, 3584 CS, The Netherlands.

Meteorology and Air Quality, Wageningen University & Research Center, Wageningen, 6708 PB, The Netherlands.

出版信息

Open Res Eur. 2022 Mar 8;1:105. doi: 10.12688/openreseurope.13875.2. eCollection 2021.

DOI:10.12688/openreseurope.13875.2
PMID:37767459
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10521041/
Abstract

A new system was developed for measuring sulfur isotopes δ S and δ S from atmospheric carbonyl sulfide (COS) on small air samples of several liters, using pre-concentration and gas chromatography - isotope ratio mass spectrometry (GC-IRMS). Measurements of COS isotopes provide a tool for quantifying the COS budget, which will help towards better understanding climate feedback mechanisms. For a 4 liter sample at ambient COS mixing ratio, ~500 parts per trillion (ppt), we obtain a reproducibility error of 2.1 ‰ for δ S and 0.4 ‰ for δ S. After applying corrections, the uncertainty for an individual ambient air sample measurement is 2.5 ‰ for δ S and 0.9 ‰ for δ S. The ability to measure small samples allows application to a global-scale sampling program with limited logistical effort. To illustrate the application of this newly developed system, we present a timeseries of ambient air measurements, during the fall and winter of 2020 and 2021 in Utrecht, the Netherlands. The observed background values were δ S = 1.0 ± 3.4 ‰ and δ S = 15.5 ± 0.8 ‰ (VCDT). The maximum observed COS mixing ratios was only 620 ppt. This, in combination with the relatively high δ S suggests that the Netherlands receives little COS-containing anthropogenic emissions. We observed a change in COS mixing ratio and δ S with different air mass origin, as modelled with HYSPLIT backward trajectory analyses. An increase of 40 ppt in mean COS mixing ratio was observed between fall and winter, which is consistent with the expected seasonal cycle in the Netherlands. Additionally, we present the results of samples from a highway tunnel to characterize vehicle COS emissions and isotopic composition. The vehicle emissions were small, with COS/CO being 0.4 ppt/ppm; the isotopic signatures are depleted relatively to background atmospheric COS.

摘要

开发了一种新系统，用于在几升小空气样本中测量来自大气羰基硫（COS）的硫同位素δ S和δ S，采用预浓缩和气相色谱 - 同位素比率质谱法（GC - IRMS）。COS同位素的测量提供了一种量化COS收支的工具，这将有助于更好地理解气候反馈机制。对于环境COS混合比约为500万亿分之一（ppt）的4升样本，我们获得的δ S的重现性误差为2.1‰，δ S的重现性误差为0.4‰。应用校正后，单个环境空气样本测量的不确定度对于δ S为2.5‰，对于δ S为0.9‰。测量小样本的能力使得能够在后勤工作有限的情况下应用于全球规模的采样计划。为了说明这个新开发系统的应用，我们展示了2020年和2021年秋冬期间在荷兰乌得勒支进行的环境空气测量的时间序列。观测到的背景值为δ S = 1.0 ± 3.4‰和δ S = 15.5 ± 0.8‰（VCDT）。观测到的最大COS混合比仅为620 ppt。这与相对较高的δ S相结合，表明荷兰几乎没有含COS的人为排放。正如用HYSPLIT反向轨迹分析所模拟的那样，我们观测到不同气团来源的COS混合比和δ S发生了变化。在秋季和冬季之间观测到平均COS混合比增加了40 ppt，这与荷兰预期的季节周期一致。此外，我们展示了来自公路隧道样本的结果，以表征车辆COS排放和同位素组成。车辆排放很小，COS/CO为0.4 ppt/ppm；同位素特征相对于背景大气COS有所贫化。

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本文引用的文献

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