Swiss halocarbon emissions for 2019 to 2020 assessed from regional atmospheric observations

Rust, D., I. Katharopoulos, M.K. Vollmer, S. Henne, S. O’Doherty, D. Say, L. Emmenegger, R. Zenobi, and S. Reimann (2022), Swiss halocarbon emissions for 2019 to 2020 assessed from regional atmospheric observations, Atmos. Chem. Phys., doi:10.5194/acp-22-2447-2022.
Abstract

Halocarbons contribute to global warming and stratospheric ozone depletion. They are emitted to the atmosphere by various anthropogenic activities. To determine Swiss national halocarbon emissions, we applied top-down methods, which rely on atmospheric concentration observations sensitive to the targeted emissions. We present 12 months (September 2019 to August 2020) of continuous atmospheric observations of 28 halocarbons from a measurement campaign at the Beromünster tall tower in Switzerland. The site is sensitive to the Swiss Plateau, which is the most densely populated area of Switzerland. Therefore, the measurements are well suited to derive Swiss halocarbon emissions. Emissions were calculated by two different top-down methods, i.e. a tracer ratio method (TRM), with carbon monoxide (CO) as the independent tracer, and a Bayesian inversion (BI), based on atmospheric transport simulations using FLEXPART–COSMO. The results were compared to previously reported top-down emission estimates, based on measurements at the high-Alpine site of Jungfraujoch, and to the bottom-up Swiss national greenhouse gas (GHG) inventory, as annually reported to the United Nations Framework Convention on Climate Change (UNFCCC). We observed moderately elevated concentrations of chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), both banned from production and consumption in Europe. The corresponding emissions are likely related to the ongoing outgassing from older foams and refrigerators and confirm the widespread historical use of these substances. For the major hydrofluorocarbons (HFCs), HFC-125 (CHF2 CF3 ) and HFC-32 (CH2 F2 ), our calculated emissions of 100 ± 34 and 45 ± 14 Mg yr−1 are in good agreement with the numbers reported in the Swiss inventory, whereas, for HFC-134a (CH2 FCF3 ), our result of 280 ± 89 Mg yr−1 is more than 30 % lower than the Swiss inventory. For HFC-152a (CH3 CHF2 ), our top-down result of 21 ± 5 Mg yr−1 is significantly higher than the number reported in the Swiss inventory. For the other investigated HFCs, perfluorocarbons (PFCs), SF6 and NF3 , Swiss emissions were small and in agreement with the inventory. Finally, we present the first country-based emission estimates for three recently phased-in, unregulated hydrofluoroolefins (HFOs), HFO-1234yf (CF3 CF=CH2 ), HFO-1234ze(E) ((E)-CF3 CH=CHF), and HCFO-1233zd(E) ((E)-CF3 CH=CHCl). For these three HFOs, we calculated Swiss emissions of 15 ± 4, 34 ± 14, and 7 ± 1 Mg yr−1 , respectively.

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Funding Sources
This research has been supported by the Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (grant no. 200020_175921). AGAGE operations are supported by the Upper Atmosphere Research Program of NASA, (grant nos. NAG5-12669, NNX07AE89G, NNX11AF17G, and NNX16AC98G to MIT; grant nos. NNX07AE87G, NNX07AF09G, NNX11AF15G, and NNX11AF16G to SIO) and the Department for Business, Energy, and Industrial Strategy (BEIS; grant no. TRN 1537/06/2018 to the University of Bristol for Mace Head and Tacolneston). Financial support for the measurements at Jungfraujoch has been provided by the Swiss National Programs HALCLIM and CLIMGAS-CH (FOEN), by the international Foundation for High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG), and by the Integrated Carbon Observation System Research Infrastructure (ICOS-CH). FLEXPART simulations were carried out at the Swiss National Supercomputing Centre (CSCS; grant nos. s862 and s1091).