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

Dominique Rust; Ioannis Katharopoulos; Martin K. Vollmer; Stephan Henne; Simon O'doherty; Daniel Say; Lukas Emmenegger; Renato Zenobi; Stefan Reimann

doi:10.5194/acp-22-2447-2022

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

Dominique Rust
, Ioannis Katharopoulos
, Martin K. Vollmer
, Stephan Henne
, Simon O'doherty
, Daniel Say
, Lukas Emmenegger
, Renato Zenobi
, Stefan Reimann^*

^*Corresponding author for this work

Research output: Contribution to journal › Article (Academic Journal) › peer-review

23 Citations (Scopus)

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 (CHF2CF3) and HFC-32 (CH2F2), our calculated emissions of 100±34 and 45±14Mgyr-1 are in good agreement with the numbers reported in the Swiss inventory, whereas, for HFC-134a (CH2FCF3), our result of 280±89Mgyr-1 is more than 30% lower than the Swiss inventory. For HFC-152a (CH3CHF2), our top-down result of 21±5Mgyr-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 (CF3CF=CH2), HFO-1234ze(E) ((E)-CF3CH=CHF), and HCFO-1233zd(E) ((E)-CF3CH=CHCl). For these three HFOs, we calculated Swiss emissions of 15±4, 34±14, and 7±1Mgyr-1, respectively.

Original language	English
Pages (from-to)	2447-2466
Number of pages	20
Journal	Atmospheric Chemistry and Physics
Volume	22
Issue number	4
DOIs	https://doi.org/10.5194/acp-22-2447-2022
Publication status	Published - 23 Feb 2022

Bibliographical note

Funding Information:
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).

Funding Information:
Financial support. This research has been supported by the Schweizerischer Nationalfonds zur Förderung der Wis-senschaftlichen 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).

Funding Information:
Acknowledgements. We thank Matthias Hill, Paul Schlauri, and Silvio Harndt from Empa, for giving fundamental instrumental and technical support. We acknowledge Rüdiger Schanda from the University of Bern, for the constructive cooperation at the Beromünster site. We acknowledge Henry Wöhrnschimmel and Sabine Schenker from the Swiss Federal Office for the Environment (FOEN), for the valuable information regarding the Swiss halocarbon consumption and the Swiss bottom-up inventory. We thank the personnel operating the Advanced Global Atmospheric Gases Experiment (AGAGE) measurement stations at Jungfraujoch, Tacolneston, and Mace Head, for conducting, evaluating, and providing the halocarbon measurement data. 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). We acknowledge the Nationales Beobachtungsnetz für Luftfremdstoffe (NABEL/FOEN; Empa), for the infrastructural contributions and for providing the carbon monoxide (CO) measurement data, and MeteoSwiss, for providing meteorological observations and COSMO model analysis. FLEXPART simulations were carried out at the Swiss National Supercomputing Centre (CSCS; grant nos. s862 and s1091). We acknowledge the Swiss National Science Foundation for funding the research for this study under the project IHALOME (SNSF; grant no. 200020_175921).

Publisher Copyright:
© 2022 Dominique Rust et al.

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SDG 12 Responsible Consumption and Production
SDG 13 Climate Action

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Cite this

@article{3dfd9b0db02640a5ad25e4a5174abdaa,

title = "Swiss halocarbon emissions for 2019 to 2020 assessed from regional atmospheric observations",

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 Berom{\"u}nster 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 (CHF2CF3) and HFC-32 (CH2F2), our calculated emissions of 100±34 and 45±14Mgyr-1 are in good agreement with the numbers reported in the Swiss inventory, whereas, for HFC-134a (CH2FCF3), our result of 280±89Mgyr-1 is more than 30\% lower than the Swiss inventory. For HFC-152a (CH3CHF2), our top-down result of 21±5Mgyr-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 (CF3CF=CH2), HFO-1234ze(E) ((E)-CF3CH=CHF), and HCFO-1233zd(E) ((E)-CF3CH=CHCl). For these three HFOs, we calculated Swiss emissions of 15±4, 34±14, and 7±1Mgyr-1, respectively.",

author = "Dominique Rust and Ioannis Katharopoulos and Vollmer, \{Martin K.\} and Stephan Henne and Simon O'doherty and Daniel Say and Lukas Emmenegger and Renato Zenobi and Stefan Reimann",

note = "Funding Information: This research has been supported by the Schweizerischer Nationalfonds zur F{\"o}rderung 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). Funding Information: Financial support. This research has been supported by the Schweizerischer Nationalfonds zur F{\"o}rderung der Wis-senschaftlichen 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). Funding Information: Acknowledgements. We thank Matthias Hill, Paul Schlauri, and Silvio Harndt from Empa, for giving fundamental instrumental and technical support. We acknowledge R{\"u}diger Schanda from the University of Bern, for the constructive cooperation at the Berom{\"u}nster site. We acknowledge Henry W{\"o}hrnschimmel and Sabine Schenker from the Swiss Federal Office for the Environment (FOEN), for the valuable information regarding the Swiss halocarbon consumption and the Swiss bottom-up inventory. We thank the personnel operating the Advanced Global Atmospheric Gases Experiment (AGAGE) measurement stations at Jungfraujoch, Tacolneston, and Mace Head, for conducting, evaluating, and providing the halocarbon measurement data. 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). We acknowledge the Nationales Beobachtungsnetz f{\"u}r Luftfremdstoffe (NABEL/FOEN; Empa), for the infrastructural contributions and for providing the carbon monoxide (CO) measurement data, and MeteoSwiss, for providing meteorological observations and COSMO model analysis. FLEXPART simulations were carried out at the Swiss National Supercomputing Centre (CSCS; grant nos. s862 and s1091). We acknowledge the Swiss National Science Foundation for funding the research for this study under the project IHALOME (SNSF; grant no. 200020\_175921). Publisher Copyright: {\textcopyright} 2022 Dominique Rust et al.",

year = "2022",

month = feb,

day = "23",

doi = "10.5194/acp-22-2447-2022",

language = "English",

volume = "22",

pages = "2447--2466",

journal = "Atmospheric Chemistry and Physics",

issn = "1680-7316",

publisher = "Copernicus Publications",

number = "4",

}

TY - JOUR

T1 - Swiss halocarbon emissions for 2019 to 2020 assessed from regional atmospheric observations

AU - Rust, Dominique

AU - Katharopoulos, Ioannis

AU - Vollmer, Martin K.

AU - Henne, Stephan

AU - O'doherty, Simon

AU - Say, Daniel

AU - Emmenegger, Lukas

AU - Zenobi, Renato

AU - Reimann, Stefan

N1 - Funding Information: 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). Funding Information: Financial support. This research has been supported by the Schweizerischer Nationalfonds zur Förderung der Wis-senschaftlichen 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). Funding Information: Acknowledgements. We thank Matthias Hill, Paul Schlauri, and Silvio Harndt from Empa, for giving fundamental instrumental and technical support. We acknowledge Rüdiger Schanda from the University of Bern, for the constructive cooperation at the Beromünster site. We acknowledge Henry Wöhrnschimmel and Sabine Schenker from the Swiss Federal Office for the Environment (FOEN), for the valuable information regarding the Swiss halocarbon consumption and the Swiss bottom-up inventory. We thank the personnel operating the Advanced Global Atmospheric Gases Experiment (AGAGE) measurement stations at Jungfraujoch, Tacolneston, and Mace Head, for conducting, evaluating, and providing the halocarbon measurement data. 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). We acknowledge the Nationales Beobachtungsnetz für Luftfremdstoffe (NABEL/FOEN; Empa), for the infrastructural contributions and for providing the carbon monoxide (CO) measurement data, and MeteoSwiss, for providing meteorological observations and COSMO model analysis. FLEXPART simulations were carried out at the Swiss National Supercomputing Centre (CSCS; grant nos. s862 and s1091). We acknowledge the Swiss National Science Foundation for funding the research for this study under the project IHALOME (SNSF; grant no. 200020_175921). Publisher Copyright: © 2022 Dominique Rust et al.

PY - 2022/2/23

Y1 - 2022/2/23

N2 - 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 (CHF2CF3) and HFC-32 (CH2F2), our calculated emissions of 100±34 and 45±14Mgyr-1 are in good agreement with the numbers reported in the Swiss inventory, whereas, for HFC-134a (CH2FCF3), our result of 280±89Mgyr-1 is more than 30% lower than the Swiss inventory. For HFC-152a (CH3CHF2), our top-down result of 21±5Mgyr-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 (CF3CF=CH2), HFO-1234ze(E) ((E)-CF3CH=CHF), and HCFO-1233zd(E) ((E)-CF3CH=CHCl). For these three HFOs, we calculated Swiss emissions of 15±4, 34±14, and 7±1Mgyr-1, respectively.

AB - 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 (CHF2CF3) and HFC-32 (CH2F2), our calculated emissions of 100±34 and 45±14Mgyr-1 are in good agreement with the numbers reported in the Swiss inventory, whereas, for HFC-134a (CH2FCF3), our result of 280±89Mgyr-1 is more than 30% lower than the Swiss inventory. For HFC-152a (CH3CHF2), our top-down result of 21±5Mgyr-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 (CF3CF=CH2), HFO-1234ze(E) ((E)-CF3CH=CHF), and HCFO-1233zd(E) ((E)-CF3CH=CHCl). For these three HFOs, we calculated Swiss emissions of 15±4, 34±14, and 7±1Mgyr-1, respectively.

UR - https://www.scopus.com/pages/publications/85125572265

U2 - 10.5194/acp-22-2447-2022

DO - 10.5194/acp-22-2447-2022

M3 - Article (Academic Journal)

AN - SCOPUS:85125572265

SN - 1680-7316

VL - 22

SP - 2447

EP - 2466

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 4

ER -

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

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