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Discussion papers
https://doi.org/10.5194/acp-2019-873
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-873
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 28 Oct 2019

Submitted as: research article | 28 Oct 2019

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

Trends and Emissions of Six Perfluorocarbons in the Northern and Southern Hemisphere

Elise S. Droste1, Karina E. Adcock1, Matthew J. Ashfold2, Charles Chou3, Zoë Fleming4,a, Paul J. Fraser5, Lauren J. Gooch1, Andrew J. Hind1, Ray L. Langenfelds5, Emma Leedham Elvidge1, Norfazrin Mohd Hanif1,6, Simon O'Doherty7, David E. Oram1,8, Chang-Feng Ou-Yang9, Marios Panagi4, Claire E. Reeves1, William T. Sturges1, and Johannes C. Laube1,10 Elise S. Droste et al.
  • 1Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK
  • 2School of Environmental and Geographical Sciences, University of Nottingham Malaysia, 43500 Semenyih, Malaysia
  • 3Research Center for Environmental Changes, Academia Sinica, Taipei 11529, Taiwan
  • 4National Centre for Atmospheric Science (NCAS), Department of Chemistry, University of Leicester, UK
  • 5Commonwealth Scientific and Industrial Research Organisation, Oceans and Atmosphere, Climate Science Centre, Aspendale, Australia
  • 6School of Environmental and Natural Resource Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia
  • 7Department of Chemistry, University of Bristol, Bristol, UK
  • 8National Centre for Atmospheric Science, School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK
  • 9Department of Atmospheric Sciences, National Central University, Taoyuan, Taiwan
  • 10Institute of Energy and Climate Research – Stratosphere (IEK-7), Forschungszentrum Jülich GmbHJ, Jülich, Germany
  • anow at: Center for Climate and Resilience Research (CR2), University of Chile, Santiago, Chile

Abstract. Perfluorocarbons (PFCs) are potent greenhouse gases with Global Warming Potentials up to several thousand times greater than CO2 on a 100-year time horizon. The lack of any significant sinks for PFCs means that they have long atmospheric lifetimes on the order of thousands of years. Anthropogenic production is thought to be the only source for most PFCs. Here we report an update on the global atmospheric abundances of the following PFCs, most of which have for the first time been separated according to their isomers: c-octafluorobutane (c-C4F8), n-decafluorobutane (n-C4F10), n-dodecafluoropentane (n-C5F12), n-tetradecafluorohexane (n-C6F14), and n-hexadecafluoroheptane (n-C7F16). Additionally, we report the first data set on the atmospheric mixing ratios of perfluoro(2-methylpentane) (i-C6F14). The existence and significance of PFC isomers has not been reported before, due to the analytical challenges of separating them. The time series spans a period from 1978 to the present. Several datasets are used to investigate temporal and spatial trends of these PFCs: time series of air samples collected at Cape Grim, Australia, from 1978 to the start of 2018; a time series of air samples collected between July 2015 and April 2017 at Tacolneston, UK; and intensive campaign-based sampling collections from Taiwan. Although the remote background Southern Hemispheric Cape Grim time series indicates that recent growth rates of most of these PFCs are lower than in the 1990s, we continue to see significantly increasing mixing ratios that are between 6 % to 27 % higher by the end of 2017 compared to abundances measured in 2010. Air samples from Tacolneston show a positive offset in PFC mixing ratios compared to the Southern Hemisphere baseline. The highest mixing ratios and variability are seen in air samples from Taiwan, which is therefore likely situated much closer to PFC sources, confirming predominantly Northern Hemispheric emissions for most PFCs. Even though these PFCs occur in the atmosphere at levels of parts per trillion molar or less, their total cumulative global emissions translate into 833 million metric tonnes of CO2 equivalent by the end of 2017, 23 % of which has been emitted in the last eight years. Almost two-thirds of the CO2 equivalent emissions are attributable to c-C4F8, which currently also has the highest emission rates that continue to grow. Despite this, the sources of all PFCs covered in this work remain poorly constrained and reported emissions in global databases do not account for the abundances found in the atmosphere.

Elise S. Droste et al.
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Elise S. Droste et al.
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Trends and Emissions of Six Perfluorocarbons in the Northern and Southern Hemisphere E. S. Droste https://doi.org/10.5281/zenodo.3519317

Elise S. Droste et al.
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Short summary
We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including...
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