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2018
Reimann, S, Elkins JW, Fraser PJ, Hall BD, Kurylo MJ, Mahieu E, Montzka SA, Prinn RG, Rigby M, Simmonds PG, Weiss RF.  2018.  Observing the atmospheric evolution of ozone-depleting substances. Comptes Rendus Geoscience. 350:384-392.   10.1016/j.crte.2018.08.008   AbstractWebsite

The atmospheric observations of ozone-depleting substances (ODSs) have been essential for following their atmospheric response to the production and use restrictions imposed by the Montreal Protocol and its Amendments and Adjustments. ODSs have been used since the first half of the 20th century in industrial and domestic applications. However, their atmospheric growth went unnoticed until the early 1970s, when they were discovered using gas chromatograph-electron capture detection (GC-ECD) instruments. Similar instrumentation formed the basis of global flask and in situ measurements commenced by NOAA and ALE/GAGE/AGAGE in the late 1970s. The combination of these networks, supported by a number of other laboratories, has been essential for following the tropospheric trends of ODSs. Additionally, ground-based remote sensing measurements within NDACC and aircraft-based observation programs have been crucial for measuring the evolution of the ODS abundances over the entire atmosphere. Maintaining these networks at least at their current state is vital for ensuring the on-going verification of the success of the Montreal Protocol. (C) 2018 Academie des sciences. Published by Elsevier Masson SAS. All rights reserved.

Vollmer, MK, Young D, Trudinger CM, Muhle J, Henne S, Rigby M, Park S, Li S, Guillevic M, Mitrevski B, Harth CM, Miller BR, Reimann S, Yao B, Steele LP, Wyss SA, Lunder CR, Arduini J, McCulloch A, Wu S, Rhee TS, Wang RHJ, Salameh PK, Hermansen O, Hill M, Langenfelds RL, Ivy D, O'Doherty S, Krummel PB, Maione M, Etheridge DM, Zhou LX, Fraser PJ, Prinn RG, Weiss RF, Simmonds PG.  2018.  Atmospheric histories and emissions of chlorofluorocarbons CFC-13 (CClF3), Sigma CFC-114 (C2Cl2F4), and CFC-115 (C2ClF5). Atmospheric Chemistry and Physics. 18:979-1002.   10.5194/acp-18-979-2018   AbstractWebsite

Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), Sigma CFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 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 mean level of 0.02 ppt yr(-1) since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. Sigma 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 8.49 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 unchanging 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 6 CFC-114 at 1.90 +/- 0.84 kt yr(-1) (similar to 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 2015-2016 are 1.14 +/- 0.50 kt yr(-1) and have doubled compared to the 2007-2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012-2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for Sigma CFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.