A fluorination method for measuring 13C-13C isotopologue of C2 molecules
A fluorination method for measuring 13C-13C isotopologue of C2 molecules
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一种测定C2分子13C-13C同位素异构体的氟化方法
DOI：
10.1002/rcm.8761
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Y.,
中科院分区：
文献类型：
--
作者：
Taguchi;K.;Yamamoto;T.;Nakagawa;M.;Gilbert;A.;Ueno;Y.,
双取代的同位素种类（“聚集”同位素）可以提供对分子的地球化学历史的见解，包括其形成温度和/或其（生物）合成途径。在这里，我们提出了一种新的测量C2分子中13 C-13 C物种的同位素比质谱仪使用传统的同位素比质谱仪。方法采用常规同位素比质谱仪，以C2 F6形式测定C2分子中的13 C-13 C同位素。乙烷和乙烯直接氟化为C2 F6。乙醇在脱水成乙烯并随后将后者脱水后测量。该方法使测量的Δ 13 C13 C值相对于一个参考工作standard.ResultsThe整个协议，包括化学修饰步骤和测量的C2 F6同位素体，是优于±0.14‰的所有化合物。天然气样品中的乙烷和生物衍生乙醇的Δ 13 C13 C值范围很窄，从0.72‰到0.90‰不等。相比之下，合成乙醇以及假定的非生物乙烷显示Δ 13 C13 C值显着不同于此范围，值分别为1.14‰和0.25‰，conclusionsThe方法提供了替代手段measurement 13 C ‐ 13 C物种，使用高分辨率质谱。来自天然和合成分子的初步数据再次强调了13 C聚集同位素物质作为（生物）标记物的潜力。
RationaleDoubly substituted isotope species (“clumped” isotopes) can provide insights into the biogeochemical history of a molecule, including its temperature of formation and/or its (bio)synthetic pathway. Here, we propose a new fluorination method for the measurement of13C‐13C species in C2molecules using a conventional isotope ratio mass spectrometer. Target molecules include ethane, ethene and ethanol.Methods13C‐13C isotope species in C2molecules were measured as C2F6using a conventional isotope ratio mass spectrometer. Ethane and ethene are directly fluorinated to C2F6. Ethanol is measured after dehydration to ethene and subsequent fluorination of the latter. The method enables the measurement of the Δ13C13C values normalized against a reference working standard.ResultsThe reproducibility of the whole protocol, including chemical modification steps and measurement of C2F6isotopologues, is better than ±0.14‰ for all the compounds. Ethane from natural gas samples and biologically derived ethanol show a narrow range of Δ13C13C values, varying from 0.72‰ to 0.90‰. In contrast, synthetic ethanol as well as putative abiotic ethane show Δ13C13C values significantly different from this range with values of 1.14‰ and 0.25‰, respectively.ConclusionsThe method presented here provides alternative means of measuring13C‐13C species to that using high‐resolution mass spectrometry. Preliminary data from natural and synthetic molecules re‐emphasizes the potential of13C clumped isotope species as a (bio)marker.