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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
https://doi.org/10.5194/acp-2017-935
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
10 Oct 2017
Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).
Atmospheric histories and emissions of chlorofluorocarbons CFC-13(CClF3), CFC-114 (C2Cl2F4), and CFC-115 (C2ClF5)
Martin K. Vollmer1, Dickon Young2, Cathy M. Trudinger3, Jens Mühle4, Stephan Henne1, Matthew Rigby2, Sunyoung Park5, Shanlan Li5, Myriam Guillevic6, Blagoj Mitrevski3, Christina M. Harth4, Benjamin R. Miller7,8, Stefan Reimann1, Bo Yao9, L. Paul Steele3, Simon A. Wyss1, Chris R. Lunder10, Jgor Arduini11,12, Archie McCulloch2, Songhao Wu5, Tae Siek Rhee13, Ray H. J. Wang14, Peter K. Salameh4, Ove Hermansen10, Matthias Hill1, Ray L. Langenfelds3, Diane Ivy15, Simon O'Doherty2, Paul B. Krummel3, Michela Maione11,12, David M. Etheridge3, Lingxi Zhou16, Paul J. Fraser3, Ronald G. Prinn15, Ray F. Weiss4, and Peter G. Simmonds2 1Laboratory for Air Pollution and Environmental Technology, Empa, Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600 Dübendorf, Switzerland
2Atmospheric Chemistry Research Group, School of Chemistry, University of Bristol, Bristol, UK
3Climate Science Centre, CSIRO Oceans and Atmosphere, Aspendale, Victoria, Australia
4Scripps Institution of Oceanography, University of California at San Diego, La Jolla, California, USA
5Kyungpook Institute of Oceanography, Kyungpook National University, South Korea
6METAS, Federal Institute of Metrology, Lindenweg 50, Bern-Wabern, Switzerland
7Earth System Research Laboratory, NOAA, Boulder, Colorado, USA
8Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
9Meteorological Observation Centre (MOC), China Meteorological Administration (CMA), Beijing, China
10Norwegian Institute for Air Research, Kjeller, Norway
11Department of Pure and Applied Sciences, University of Urbino, Urbino, Italy
12Institute of Atmospheric Sciences and Climate, Italian National Research Council, Bologna, Italy
13Korea Polar Research Institute, KIOST, Incheon, South Korea
14School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA
15Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
16Chinese Academy of Meteorological Sciences (CAMS), China Meteorological Administration (CMA), Beijing, China
Abstract. Based on observations of three chlorofluorocarbons, CFC-13 (chlorotrifluoromethane), CFC-114 (dichlorotetrafluoroethane) and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly eight decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in-situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry air mole fraction in parts-per-trillion, pmol mol−-1) in 2016. Its growth rate has decreased since the mid 1980s but has remained at a surprisingly high level of 0.02 ppt yr−1 since the late 2000s. CFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s, and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.52 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unaltered lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: Mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of CFC-114 at 1.90 ± 0.84 kt yr−1 (~ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2014–2016 are 1.08 ± 0.50 kt yr−1 and have more than doubled compared to 2009. Cumulative global emissions for CFC-114 derived from observations through 2016 exceed the global cumulative production derived from reported inventory data by > 10 % while those for CFC-115 agree well. We find CFC-13 emissions from aluminum smelters and impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions neither of them can account for the lingering global emissions determined from the atmospheric observations. We also conduct regional inversions for the years 2012–2016 for the north-east Asian area using observations from the Korean Gosan AGAGE site and find significant emissions for CFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in north-eastern Asia and more specifically on the Chinese mainland.

Citation: Vollmer, M. K., Young, D., Trudinger, C. M., Mühle, J., Henne, S., Rigby, M., Park, S., Li, S., Guillevic, M., Mitrevski, B., Harth, C. M., Miller, B. R., Reimann, S., Yao, B., Steele, L. P., Wyss, S. A., Lunder, C. R., Arduini, J., McCulloch, A., Wu, S., Rhee, T. S., Wang, R. H. J., Salameh, P. K., Hermansen, O., Hill, M., Langenfelds, R. L., Ivy, D., O'Doherty, S., Krummel, P. B., Maione, M., Etheridge, D. M., Zhou, L., Fraser, P. J., Prinn, R. G., Weiss, R. F., and Simmonds, P. G.: Atmospheric histories and emissions of chlorofluorocarbons CFC-13(CClF3), CFC-114 (C2Cl2F4), and CFC-115 (C2ClF5), Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-935, in review, 2017.
Martin K. Vollmer et al.
Martin K. Vollmer et al.
Martin K. Vollmer et al.

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Short summary
We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere because they are important in stratospheric ozone depletion. These compounds should have decreased in the atmosphere because their are banned by the Montreal Protocol but we find the opposite, Emissions over the last decade have increased on a global scale. We use inverse modeling and our observations to find that a large part of the emissions in the Asian region.
We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere...
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