Atmospheric abundance and global emissions of perfluorocarbons CF4, C2F6 and C3F8 since 1800 inferred from ice core, firn, air archive and in situ measurements

• Published in: Atmospheric Chemistry and Physics
• Main Authors: Trudinger, Cathy M., Fraser, Paul J., Etheridge, David M., Sturges, William T., Vollmer, Martin K., Rigby, Matt, Martinerie, Patricia, Mühle, Jens, Worton, David R., Krummel, Paul B., Steele, L. Paul, Miller, Benjamin R., Laube, Johannes, Mani, Francis S., Rayner, Peter J., Harth, Christina M., Witrant, Emmanuel, Blunier, Thomas, Schwander, Jakob, O'Doherty, Simon, Battle, Mark
• Other Authors: CSIRO Marine and Atmospheric Research (CSIRO-MAR), Commonwealth Scientific and Industrial Research Organisation Canberra (CSIRO), University of East Anglia Norwich (UEA), Swiss Federal Laboratories for Materials Science and Technology Dübendorf (EMPA), University of Bristol Bristol, Institut des Géosciences de l’Environnement (IGE), Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ), University of California San Diego (UC San Diego), University of California (UC), National Physical Laboratory Teddington (NPL), University of Colorado Boulder, University of the South Pacific (USP), University of Melbourne, GIPSA - Systèmes linéaires et robustesse (GIPSA-SLR), Département Automatique (GIPSA-DA), Grenoble Images Parole Signal Automatique (GIPSA-lab ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Grenoble Images Parole Signal Automatique (GIPSA-lab ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ), Centre for Ice and Climate Copenhagen, Niels Bohr Institute Copenhagen (NBI), Faculty of Science Copenhagen, University of Copenhagen = Københavns Universitet (UCPH)-University of Copenhagen = Københavns Universitet (UCPH)-Faculty of Science Copenhagen, University of Copenhagen = Københavns Universitet (UCPH)-University of Copenhagen = Københavns Universitet (UCPH), Universität Bern = University of Bern = Université de Berne (UNIBE), Department of Physics and Astronomy Brunswick, Bowdoin College Brunswick
• Format: Article in Journal/Newspaper
• Language: English
• Published: HAL CCSD 2016
• Subjects: [SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology; ice core; South pole
• Online Access: https://hal.univ-grenoble-alpes.fr/hal-01411370; https://hal.univ-grenoble-alpes.fr/hal-01411370/document; https://hal.univ-grenoble-alpes.fr/hal-01411370/file/acp-16-11733-2016.pdf; https://doi.org/10.5194/acp-16-11733-2016

International audience Perfluorocarbons (PFCs) are very potent and long-lived greenhouse gases in the atmosphere, released predominantly during aluminium production and semiconductor manufacture. They have been targeted for emission controls under the United Nations Framework Convention on Climate Change. Here we present the first continuous records of the atmospheric abundance of CF4 (PFC-14), C2F6 (PFC-116) and C3F8 (PFC-218) from 1800 to 2014. The records are derived from high-precision measurements of PFCs in air extracted from polar firn or ice at six sites (DE08, DE08-2, DSSW20K, EDML, NEEM and South Pole) and air archive tanks and atmospheric air sampled from both hemispheres. We take account of the age characteristics of the firn and ice core air samples and demonstrate excellent consistency between the ice core, firn and atmospheric measurements. We present an inversion for global emissions from 1900 to 2014. We also formulate the inversion to directly infer emission factors for PFC emissions due to aluminium production prior to the 1980s. We show that 19th century atmospheric levels, before significant anthropogenic influence, were stable at 34.1 ± 0.3 ppt for CF4 and below detection limits of 0.002 and 0.01 ppt for C2F6 and C3F8, respectively. We find a significant peak in CF4 and C2F6 emissions around 1940, most likely due to the high demand for aluminium during World War II, for example for construction of aircraft, but these emissions were nevertheless much lower than in recent years. The PFC emission factors for aluminium production in the early 20th century were significantly higher than today but have decreased since then due to improvements and better control of the smelting process. Mitigation efforts have led to decreases in emissions from peaks in 1980 (CF4) or early-to-mid-2000s (C2F6 and C3F8) despite the continued increase in global aluminium production; however, these decreases in emissions appear to have recently halted. We see a temporary reduction of around 15 % in CF4 emissions in ...