A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021

Martin Vojta; Andreas Plach; Saurabh Annadate; Sunyoung Park; Gawon Lee; Pallav Purohit; Florian Lindl; Xin Lan; Jens Mühle; Rona L. Thompson; Andreas Stohl

doi:10.5194/acp-24-12465-2024

A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021

Martin Vojta (Corresponding author)
, Andreas Plach
, Saurabh Annadate
, Sunyoung Park
, Gawon Lee
, Pallav Purohit
, Florian Lindl
, Xin Lan
, Jens Mühle
, Rona L. Thompson
, Andreas Stohl

Department of Meteorology and Geophysics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.

Original language	English
Pages (from-to)	12465-12493
Number of pages	29
Journal	Atmospheric Chemistry and Physics
Volume	24
Issue number	21
DOIs	https://doi.org/10.5194/acp-24-12465-2024
Publication status	Published - 11 Nov 2024

Funding

We thank the whole AGAGE team for providing measurement data, including Christina M. Harth, Jens M\u00FChle, Peter K. Salameh, and Ray F.Weiss (Scripps Institution of Oceanography, UCSD); Paul B. Krummel, Paul J. Fraser, and Paul Steele (CSIRO Environment); Hsiang-Jui (Ray) Wang (Georgia Institute of Technology); Simon O'Doherty, Dickon Young, and Kieran M. Stanley (University of Bristol); Martin K. Vollmer and Stefan Reimann (Empa, Swiss Federal Laboratories for Materials Science and Technology); and Chris Rene Lunder and Ove Hermanson (NILU, Norwegian Institute for Air Research), and particularly all station managers and station operators. AGAGE operations at Mace Head, Trinidad Head, Cape Matatula, Ragged Point, and Kennaook / Cape Grim are supported by NASA (USA) grants to MIT (grant nos. NAG5- 12669, NNX07AE89G, NNX11AF17G, and NNX16AC98G) and SIO (grant nos. NNX07AE87G, NNX07AF09G, NNX11AF15G, NNX11AF16G, NNX16AC96G, and NNX16AC97G) and also by the Department for Business, Energy and Industrial Strategy (BEIS, UK) under contract no. 5488/11/2021 to the University of Bristol for Mace Head and NOAA (USA); under contract no. 1305M319CNRMJ0028 to the University of Bristol for Ragged Point; CSIRO, BoM, DCCEEW, and RRA (Australia); NILU (Norway); KNU (Korea); CMA (China); NIES (Japan); and Urbino University (Italy). For Jungfraujoch, funding is acknowledged for the project of HALCLIM/CLIMGAS-CH by the Swiss Federal Office for the Environment (FOEN) and for ICOS (Integrated Carbon Observation System) by the Swiss National Science Foundation. In addition, measurements are supported by the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG). The Commonwealth Scientific and Industrial Research Organisation (CSIRO, Australia) and Bureau of Meteorology (Australia) are thanked for their ongoing long-term support and funding of the Kennaook / Cape Grim station and the Kennaook / Cape Grim science programme. Operations of the Gosan station on Jeju Island, South Korea, were supported by the National Research Foundation of Korea grant funded by the South Korean government MSIT (grant no. RS-2023-00229318). We also thank the NOAA Global Monitoring Laboratory for providing access to their data, including Geoff Dutton, James W. Elkins, Fred Moore, Eric Hintsa, Dale Hurst, Bradley Hall, Kathryn McKain, Stephen Montzka, John Bharat Miller, Colm Sweeney, Ed Dlugokencky, Arlyn Andrews, David Nance, and Christina M. Harth and the key partners Le Huang (EC) and Kenneth Davis (PSU). Observations collected in the Southern Great Plains (SGP) by S\u00E9bastien Biraud (Lawrence Berkeley National Laboratory, USA) were supported by the Office of Biological and Environmental Research of the U.S. Department of Energy under contract no. DE-AC02-05CH11231 as part of the Atmospheric Radiation Measurement Program (ARM) and Environmental System Science (ESS) Program. We further acknowledge the following people and institutions for sharing their observation data: Takuya Saito (National Institute for Environmental Studies, Japan), Emilio Cuevas (State Meteorological Agency, Spain), Dan Say (University of Bristol), Jgor Arduini (University of Urbino), Cedric Couret (German Environment Agency), Elena Popa (Utrecht University), Satoshi Sugawara (Miyagi University of Education, Japan), Armin Rauthe and Jonathan Williams (Max Planck Institute for Chemistry), Tanja Schuck (Goethe University Frankfurt), Florian Obersteiner (Karlsruhe Institute of Technology), and Luciana Vanni Gatti (Instituto Nacional de Pesquisas Espaciais). The computational results presented have been achieved in part using the Vienna Scientific Cluster (VSC), project no. 71878, demonstration of a Lagrangian re-analysis, for which we are grateful. We further acknowledgement the use of ECMWF's computing and archive facilities provided through a special project (spatvojt) in this research. The study has been supported by EYECLIMA, a European Union Horizon Europe research and innovation programme under grant no. 101081395. We thank Lei Hu and Christina Groot Zwaaftink for the discussions. We also thank Marina D\u00FCtsch, Lucie Bakels, Silvia Bucci, Katharina Baier, Daria Tatsii, Anjumol Raju, Rakesh Subramanian, Sophie Wittig, Omid Nabavi, Ioanna Evangelou, Michael Blaschek, Andrey Skorokhod, and Petra Seibert (University of Vienna) for their support. Finally, we want to thank Matthew Toohey for editing our paper and the two anonymous reviewers for their constructive comments, which substantially improved our work. The computational results presented have been achieved in part using the Vienna Scientific Cluster (VSC), project no. 71878, demonstration of a Lagrangian re-analysis, for which we are grateful. We further acknowledgement the use of ECMWF's computing and archive facilities provided through a special project (spatvojt) in this research. The study has been supported by EYE-CLIMA, a European Union Horizon Europe research and innovation programme under grant no. 101081395. We thank Lei Hu and Christina Groot Zwaaftink for the discussions. We also thank Marina D\u00FCtsch, Lucie Bakels, Silvia Bucci, Katharina Baier, Daria Tatsii, Anjumol Raju, Rakesh Subramanian, Sophie Wittig, Omid Nabavi, Ioanna Evangelou, Michael Blaschek, Andrey Skorokhod, and Petra Seibert (University of Vienna) for their support. Finally, we want to thank Matthew Toohey for editing our paper and the two anonymous reviewers for their constructive comments, which substantially improved our work. We thank the whole AGAGE team for providing measurement data, including Christina M. Harth, Jens M\u00FChle, Peter K. Salameh, and Ray F. Weiss (Scripps Institution of Oceanography, UCSD); Paul B. Krummel, Paul J. Fraser, and Paul Steele (CSIRO Environment); Hsiang-Jui (Ray) Wang (Georgia Institute of Technology); Simon O'Doherty, Dickon Young, and Kieran M. Stanley (University of Bristol); Martin K. Vollmer and Stefan Reimann (Empa, Swiss Federal Laboratories for Materials Science and Technology); and Chris Rene Lunder and Ove Hermanson (NILU, Norwegian Institute for Air Research), and particularly all station managers and station operators. AGAGE operations at Mace Head, Trinidad Head, Cape Matatula, Ragged Point, and Kennaook / Cape Grim are supported by NASA (USA) grants to MIT (grant nos. NAG5-12669, NNX07AE89G, NNX11AF17G, and NNX16AC98G) and SIO (grant nos. NNX07AE87G, NNX07AF09G, NNX11AF15G, NNX11AF16G, NNX16AC96G, and NNX16AC97G) and also by the Department for Business, Energy and Industrial Strategy (BEIS, UK) under contract no. 5488/11/2021 to the University of Bristol for Mace Head and NOAA (USA); under contract no. 1305M319CNRMJ0028 to the University of Bristol for Ragged Point; CSIRO, BoM, DCCEEW, and RRA (Australia); NILU (Norway); KNU (Korea); CMA (China); NIES (Japan); and Urbino University (Italy). For Jungfraujoch, funding is acknowledged for the project of HALCLIM/CLIMGAS-CH by the Swiss Federal Office for the Environment (FOEN) and for ICOS (Integrated Carbon Observation System) by the Swiss National Science Foundation. In addition, measurements are supported by the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG). The Commonwealth Scientific and Industrial Research Organisation (CSIRO, Australia) and Bureau of Meteorology (Australia) are thanked for their ongoing long-term support and funding of the Kennaook / Cape Grim station and the Kennaook / Cape Grim science programme. Operations of the Gosan station on Jeju Island, South Korea, were supported by the National Research Foundation of Korea grant funded by the South Korean government MSIT (grant no. RS-2023-00229318). We also thank the NOAA Global Monitoring Laboratory for providing access to their data, including Geoff Dutton, James W. Elkins, Fred Moore, Eric Hintsa, Dale Hurst, Bradley Hall, Kathryn McKain, Stephen Montzka, John Bharat Miller, Colm Sweeney, Ed Dlugokencky, Arlyn Andrews, David Nance, and Christina M. Harth and the key partners Le Huang (EC) and Kenneth Davis (PSU). Observations collected in the Southern Great Plains (SGP) by S\u00E9bastien Biraud (Lawrence Berkeley National Laboratory, USA) were supported by the Office of Biological and Environmental Research of the U.S. Department of Energy under contract no. DE\u2010AC02\u201005CH11231 as part of the Atmospheric Radiation Measurement Program (ARM) and Environmental System Science (ESS) Program.

Austrian Fields of Science 2012

105206 Meteorology

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https://phaidra.univie.ac.at/o:2156156Licence: CC BY 4.0

Cite this

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title = "A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021",

abstract = "We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.",

author = "Martin Vojta and Andreas Plach and Saurabh Annadate and Sunyoung Park and Gawon Lee and Pallav Purohit and Florian Lindl and Xin Lan and Jens M{\"u}hle and Thompson, \{Rona L.\} and Andreas Stohl",

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AU - Vojta, Martin

AU - Plach, Andreas

AU - Annadate, Saurabh

AU - Park, Sunyoung

AU - Lee, Gawon

AU - Purohit, Pallav

AU - Lindl, Florian

AU - Lan, Xin

AU - Mühle, Jens

AU - Thompson, Rona L.

AU - Stohl, Andreas

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N2 - We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.

AB - We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.

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JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

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A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021

Abstract

Funding

Austrian Fields of Science 2012

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