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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
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https://doi.org/10.5194/acp-2020-843
https://doi.org/10.5194/acp-2020-843

  11 Sep 2020

11 Sep 2020

Review status: a revised version of this preprint is currently under review for the journal ACP.

Stratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12 and CFC-113 isotopologues

Max Thomas1, Johannes C. Laube1,2, Jan Kaiser1, Samuel Allin1, Patricia Martinerie3, Robert Mulvaney4, Anna Ridley1, Thomas Röckmann5, William T. Sturges1, and Emmanuel Witrant6 Max Thomas et al.
  • 1Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich
  • 2Institute of Energy and Climate Research – Stratosphere (IEK-7), Forschungszentrum Jülich GmbHJ, Jülich, Germany
  • 3Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, IGE, 38000 Grenoble, France
  • 4British Antarctic Survey, Cambridge, UK
  • 5Institute for Marine and Atmospheric Research, Utrecht University, Utrecht, the Netherlands
  • 6Université Grenoble Alpes, CNRS, Grenoble Image Parole Signal Automatique (GIPSA-Lab), Grenoble, France

Abstract. We present novel measurements of the carbon isotope composition of CFC-11 (CCl3F), CFC-12 (CCl2F2), and CFC-113 (CF2ClCFCl2), three atmospheric trace gases that are important for both stratospheric ozone depletion and global warming. These measurements were carried out on air samples collected in the stratosphere – the main sink region for these gases – and on air extracted from deep polar firn snow. We quantify, for the first time, the apparent isotopic fractionation, εapp(13C), for these gases as they are destroyed in the high- and mid-latitude stratosphere: εapp(CFC-12, high-lat) = (−20.2 ± 4.4) ‰ and εapp(CFC-113, high-lat) = (−9.4 ± 4.4) ‰, εapp(CFC-12, mid-lat) = (−30.3 ± 10.7) ‰, and εapp(CFC-113, mid-lat) = (−34.4 ± 9.8) ‰. Our CFC-11 measurements were not sufficient to calculate εapp(CFC-11) so we instead used previously reported photolytic fractionation for CFC-11 and CFC-12 to scale our εapp(CFC-12), resulting in εapp(CFC-11, high-lat) = (−7.8 ± 1.7) ‰ and εapp(CFC-11, mid-lat) = (−11.7 ± 4.2) ‰. Measurements of firn air were used to construct histories of the tropospheric isotopic composition, δT(13C), for CFC-11 (1950s to 2009), CFC-12 (1950s to 2009), and CFC-113 (1970s to 2009) – with δT(13C) increasing for each gas. We used εapp(high-lat), which were derived from more data, and a constant isotopic composition of emissions, δE(13C), to model δT(13C, CFC-11), δT(13C, CFC-12), and δT(13C, CFC-113). For CFC-11 and CFC-12, modelled δT(13C) was consistent with measured δT(13C) for the entire period covered by the measurements, suggesting no dramatic change in δE(13C, CFC-11) or δE(13C, CFC-12) has occurred since the 1950s. For CFC-113, our modelled δT(13C, CFC-113) did not agree with our measurements earlier than 1980. While this discrepancy may be indicative of a change in δE(13C, CFC-113), it is premature to assign one. Our modelling predicts increasing δT(13C, CFC-11), δT(13C, CFC-12), and δT(13C, CFC-113) into the future. We investigated the effect of recently reported new CFC-11 emissions on background δT(13C, CFC-11) by fixing model emissions after 2012, and comparing δT(13C, CFC-11) in this scenario to the model base case. The difference in δT(13C, CFC-11) between these scenarios was 1.4 ‰ in 2050. This difference is smaller than our model uncertainty envelope and would therefore require improved modelling and measurement precision, as well as better quantified isotopic source compositions, to detect.

Max Thomas et al.

 
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Max Thomas et al.

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Short summary
CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
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