Atmos. Chem. Phys. Discuss., 12, 4073-4100, 2012
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Distributions, long term trends and emissions of four perfluorocarbons in remote parts of the atmosphere and firn air
J. C. Laube1, C. Hogan1, M. J. Newland1, F. S. Mani1,2, P. J. Fraser3, C. A. M. Brenninkmeijer4, P. Martinerie5, D. E. Oram6, T. Röckmann7, J. Schwander8, E. Witrant9, G. P. Mills1, C. E. Reeves1, and W. T. Sturges1
1School of Environmental Sciences, University of East Anglia, Norwich, UK
2School of Applied Sciences, Fiji National University, Suva, Fiji
3Centre for Australian Weather and Climate Research, Commonwealth Scientific and Industrial Research Organisation, Aspendale, Victoria 3195, Australia
4Max Planck Institute for Chemistry, Air Chemistry Division, Mainz, Germany
5UJF – Grenoble 1/CNRS, Laboratoire de Glaciologie et Géophysique de l'Environnement (LGGE) UMR 5183, Grenoble, 38041, France
6National Centre for Atmospheric Science, School of Environmental Sciences, University of East Anglia, Norwich, UK
7Institute for Marine and Atmospheric Research, Utrecht University, Utrecht, The Netherlands
8Physics Institute, University of Berne, Bern, Switzerland
9UJF – Grenoble 1/CNRS, Grenoble Image Parole Signal Automatique (GIPSA-lab), UMR 5216, B.P. 46, 38402 St Martin d'Hères, France

Abstract. We report the first data set of atmospheric abundances for the following four perfluoroalkanes: n-decafluorobutane (n-C4F10), n-dodecafluoropentane (n-C5F12), n-tetradecafluorohexane (n-C6F14) and n-hexadecafluoroheptane (n-C7F16). All four compounds could be detected and quantified in air samples from remote locations in the Southern Hemisphere (at Cape Grim, Tasmania, archived samples dating back to 1978) and the upper troposphere (a passenger aircraft flying from Germany to South Africa). Further observations originate from air samples extracted from deep firn in Greenland and allow trends of atmospheric abundances in the earlier 20th century to be inferred. All four compounds were not present in the atmosphere prior to the 1960s. n-C4F10 and n-C5F12 were also measured in samples collected in the stratosphere confirming their very long atmospheric lifetimes. Emissions were inferred from these observations and found to be comparable with emissions from the EDGAR database for n-C6F14. However, emissions of n-C4F10, n-C5F12 and n-C7F16 were found to differ by up to five orders of magnitude. Although the abundances of the four perfluorocarbons reported here are currently small (less than 0.3 ppt, parts per trillion) they have strong Global Warming Potentials several thousand times higher than carbon dioxide and continue to increase in the atmosphere. The sum of their cumulative emissions reached 325 mt (million metric tonnes) CO2 equivalent at the end of 2009.

Citation: Laube, J. C., Hogan, C., Newland, M. J., Mani, F. S., Fraser, P. J., Brenninkmeijer, C. A. M., Martinerie, P., Oram, D. E., Röckmann, T., Schwander, J., Witrant, E., Mills, G. P., Reeves, C. E., and Sturges, W. T.: Distributions, long term trends and emissions of four perfluorocarbons in remote parts of the atmosphere and firn air, Atmos. Chem. Phys. Discuss., 12, 4073-4100, doi:10.5194/acpd-12-4073-2012, 2012.
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