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Absolute isotope ratios of carbon dioxide – a feasibility study
Journal of Analytical Atomic Spectrometry ( IF 3.1 ) Pub Date : 2020-09-09 , DOI: 10.1039/d0ja00318b
Lukas Flierl 1, 2, 3 , Olaf Rienitz 1, 2, 3 , Paul J. Brewer 4, 5, 6, 7 , Harro A. J. Meijer 8, 9, 10, 11, 12 , Farilde M. Steur 8, 9, 10, 11, 12
Affiliation  

One way of obtaining isotope ratios, traceable to the International System of Units, is the gravimetric isotope mixtures method. Adapting this method to carbon dioxide is challenging since measuring all twelve isotopologues at once with a gas mass spectrometer is currently not possible. The calculation of the mass bias correction factors is no straightforward task due to the fact that the isotopic equilibrium has to be considered. This publication demonstrates a potential way of adapting this method to carbon dioxide while considering isotope equilibrium. We also show how we prepared binary blends from enriched/depleted carbon dioxide parent gases and how equilibrating the different gases by heating affects the measurements. Furthermore, we reveal mathematical limitations of our approach when the gases are not in isotope equilibrium and which issues occur due to measurement limitations. In a simulation, using authentic data, we asses our approach in terms of achievable uncertainties and discuss further improvements, like using atomic spectroscopy methods.

中文翻译:

二氧化碳的绝对同位素比–可行性研究

可溯源到国际单位制的一种获取同位素比率的方法是重量同位素混合物法。使这种方法适应二氧化碳是具有挑战性的,因为目前无法使用气体质谱仪同时测量所有十二种同位素。由于必须考虑同位素平衡的事实,质量偏差校正因子的计算不是直接的任务。该出版物证明了在考虑同位素平衡的同时使该方法适应二氧化碳的潜在方法。我们还展示了如何从富集/耗尽的二氧化碳母气中制备二元混合物,以及如何通过加热来平衡不同气体对测量的影响。此外,我们揭示了当气体不处于同位素平衡状态并且由于测量限制而发生哪些问题时我们方法的数学局限性。在模拟中,使用真实数据,我们根据可实现的不确定性评估了我们的方法,并讨论了进一步的改进,例如使用原子光谱法。
更新日期:2020-11-03
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