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Discussion papers
https://doi.org/10.5194/acp-2018-852
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-852
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 25 Sep 2018

Research article | 25 Sep 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Abundances, emissions, and loss processes of the long-lived and potent greenhouse gas octafluorooxolane (octafluorotetrahydrofuran, c-C4F8O) in the atmosphere

Martin K. Vollmer1, François Bernard2,3,4, Blagoj Mitrevski5, L. Paul Steele5, Cathy M. Trudinger5, Stefan Reimann1, Ray L. Langenfelds5, Paul B. Krummel5, Paul J. Fraser5, David M. Etheridge5, Marc A. J. Curran6,7, and James B. Burkholder2 Martin K. Vollmer et al.
  • 1Laboratory for Air Pollution and Environmental Technology, Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
  • 2Earth System Research Laboratory, NOAA, National Oceanic and Atmospheric Administration, Boulder, Colorado, USA
  • 3Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
  • 4now at: Institut de Combustion Aérothermique, Réactivité et Environnement, Centre National de la Recherche Scientifique, Observatoire des Sciences de l’Univers en région Centre, Orléans, France
  • 5Climate Science Centre, CSIRO Oceans and Atmosphere, Aspendale, Victoria, Australia
  • 6Australian Antarctic Division, 203 Channel Highway, Kingston, Tasmania 7050, Australia
  • 7Antarctic Climate & Ecosystems Cooperative Research Centre, Hobart, Tasmania 7001, Australia

Abstract. The first observations of octafluorooxolane (octafluorotetrahydrofuran, c-C4F8O), a persistent greenhouse gas, in the atmosphere are reported. In addition, a complimentary laboratory study of its most likely atmospheric loss processes and infrared absorption spectrum and global warming potential (GWP) are reported. First atmospheric measurements of c-C4F8O are provided from the Cape Grim Air Archive (41°S, Tasmania, Australia, 1978–present), supplemented by two firn air samples from Antarctica, in situ measurements of ambient air at Aspendale, Victoria (38°S), and a few archived air samples from the Northern Hemisphere. Atmospheric abundances in the Southern Hemisphere have reached 74ppq (parts per quadrillion, femtomolmol-1 in dry air) by 2017. However its growth rate has decreased from a maximum in 2004 of 4.3ppqyr-1 to <0.15ppqyr-1 in 2017. Using a 12-box atmospheric transport model, globally averaged yearly emissions and abundances of c-C4F8O are calculated for 1951–2017. Emissions, which we speculate to derive predominantly from usage of c-C4F8O as a solvent in the semiconductor industry, peaked at 0.16 (±0.04, 2σ)ktyr-1 in 2004 and have after declined to <0.01ktyr-1 in 2017. Cumulative emissions over the full range of our record amount to 2.8 (2.6–3.2)kt, which correspond to 34Mt of CO2-equivalent emissions. Infrared and ultraviolet absorption spectra for c-C4F8O as well as the reactive channel rate coefficient for the O(1D)+c-C4F8O reaction was determined from laboratory studies. On the basis of these experiments, a radiative efficiency of 0.430Wm-2ppb-1 (parts per billion, nanomolmol-1) was determined, which is one of the largest found for synthetic greenhouse gases. The global annually averaged atmospheric lifetime, including mesospheric loss, is estimated to be >3000 years. GWPs of 8975, 12000, and 16000 are estimated for the 20, 100, and 500-year time-horizons, respectively.

Martin K. Vollmer et al.
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Short summary
We have discovered a new compound in the atmosphere. We find that this compound, with the complicated name 'octafluorooxolane (c-C4F8O), turns out to be a very powerful greenhouse gas thereby contributing to global warming, and that it has a very long atmospheric lifetime of more than 3500 years. We measured c-C4F8O in old air samples and could reconstruct its atmospheric evolution. Based on this, we could estimate the global emissions of c-C4F8O to the atmosphere.
We have discovered a new compound in the atmosphere. We find that this compound, with the...
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