Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China

Haklim Choi; Mi Kyung Park; Paul J. Fraser; Hyeri Park; Sohyeon Geum; Jens Mühle; Jooil Kim; Ian Porter; Peter K. Salameh; Christina M. Harth; Bronwyn L. Dunse; Paul B. Krummel; Ray F. Weiss; Simon O'Doherty; Dickon Young; Sunyoung Park

doi:10.5194/acp-22-5157-2022

Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China

Haklim Choi, Mi Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, Sunyoung Park^*

^*Corresponding author for this work

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

15 Citations (Scopus)

Abstract

Methyl bromide (CH3Br) is a potent ozone-depleting substance (ODS) that has both natural and anthropogenic sources. CH3Br has been used mainly for preplant soil fumigation, post-harvest grain and timber fumigation, and structural fumigation. Most non-quarantine and pre-shipment (non-QPS) uses were phased out by 2005 for non-Article 5 (developed) countries and by 2015 for Article 5 (developing) countries under the Montreal Protocol on Substances that Deplete the Ozone Layer; some uses have continued under critical-use exemptions (CUEs). Under the protocol, individual nations are required to report annual data on CH3Br production and consumption for quarantine-pre-shipment (QPS) uses, non-QPS uses, and CUEs to the United Nations Environment Programme (UNEP). In this study, we analyzed high-precision, in situ measurements of atmospheric mole fractions of CH3Br obtained at the Gosan station on Jeju Island, South Korea, from 2008 to 2019. The background mole fractions of CH3Br in the atmosphere at Gosan declined from 8.5±0.8gppt (parts per trillion) in 2008 to 7.4±0.6gppt in 2019 at a rate of -0.13±0.02gpptgyr-1. At Gosan, we also observed periods of persistent mole fractions (pollution events) elevated above the decreasing background in continental air masses from China. Statistical back-trajectory analyses showed that these pollution events are predominantly traced back to CH3Br emissions from eastern China. Using an interspecies correlation (ISC) method with the reference trace species CFC-11 (CCl3F), we estimate anthropogenic CH3Br emissions from eastern China at an average of 4.1±1.3gGggyr-1 in 2008-2019, approximately 2.9±1.3gGggyr-1 higher than the bottom-up emission estimates reported to UNEP. Possible non-fumigation CH3Br sources - rapeseed production and biomass burning - were assessed, and it was found that the discrepancy is most likely due to unreported or incorrectly reported QPS and non-QPS fumigation uses. These unreported anthropogenic emissions of CH3Br are confined to eastern China and account for 30g%-40g% of anthropogenic global CH3Br emissions. They are likely due to delays in the introduction of CH3Br alternatives, such as sulfuryl fluoride (SO2F2), heat, and irradiation, and a possible lack of industry awareness of the need for regulation of CH3Br production and use.

Original language	English
Pages (from-to)	5157-5173
Number of pages	17
Journal	Atmospheric Chemistry and Physics
Volume	22
Issue number	8
DOIs	https://doi.org/10.5194/acp-22-5157-2022
Publication status	Published - 20 Apr 2022

Bibliographical note

Funding Information:
Financial support. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University.

Funding Information:
This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens M?hle, Christina M. Harth, Peter K. Salameh, and Ray F.Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University.

Funding Information:
Acknowledgements. This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens Mühle, Christina M. Harth, Peter K. Salameh, and Ray F. Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University.

Publisher Copyright:
© 2022 Haklim Choi et al.

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Choi, H., Park, M. K., Fraser, P. J., Park, H., Geum, S., Mühle, J., Kim, J., Porter, I., Salameh, P. K., Harth, C. M., Dunse, B. L., Krummel, P. B., Weiss, R. F., O'Doherty, S., Young, D., & Park, S. (2022). Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China. Atmospheric Chemistry and Physics, 22(8), 5157-5173. https://doi.org/10.5194/acp-22-5157-2022

@article{3e41221b2c364e5db637e24a0a8a3888,

title = "Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China",

abstract = "Methyl bromide (CH3Br) is a potent ozone-depleting substance (ODS) that has both natural and anthropogenic sources. CH3Br has been used mainly for preplant soil fumigation, post-harvest grain and timber fumigation, and structural fumigation. Most non-quarantine and pre-shipment (non-QPS) uses were phased out by 2005 for non-Article 5 (developed) countries and by 2015 for Article 5 (developing) countries under the Montreal Protocol on Substances that Deplete the Ozone Layer; some uses have continued under critical-use exemptions (CUEs). Under the protocol, individual nations are required to report annual data on CH3Br production and consumption for quarantine-pre-shipment (QPS) uses, non-QPS uses, and CUEs to the United Nations Environment Programme (UNEP). In this study, we analyzed high-precision, in situ measurements of atmospheric mole fractions of CH3Br obtained at the Gosan station on Jeju Island, South Korea, from 2008 to 2019. The background mole fractions of CH3Br in the atmosphere at Gosan declined from 8.5±0.8gppt (parts per trillion) in 2008 to 7.4±0.6gppt in 2019 at a rate of -0.13±0.02gpptgyr-1. At Gosan, we also observed periods of persistent mole fractions (pollution events) elevated above the decreasing background in continental air masses from China. Statistical back-trajectory analyses showed that these pollution events are predominantly traced back to CH3Br emissions from eastern China. Using an interspecies correlation (ISC) method with the reference trace species CFC-11 (CCl3F), we estimate anthropogenic CH3Br emissions from eastern China at an average of 4.1±1.3gGggyr-1 in 2008-2019, approximately 2.9±1.3gGggyr-1 higher than the bottom-up emission estimates reported to UNEP. Possible non-fumigation CH3Br sources - rapeseed production and biomass burning - were assessed, and it was found that the discrepancy is most likely due to unreported or incorrectly reported QPS and non-QPS fumigation uses. These unreported anthropogenic emissions of CH3Br are confined to eastern China and account for 30g\%-40g\% of anthropogenic global CH3Br emissions. They are likely due to delays in the introduction of CH3Br alternatives, such as sulfuryl fluoride (SO2F2), heat, and irradiation, and a possible lack of industry awareness of the need for regulation of CH3Br production and use.",

author = "Haklim Choi and Park, \{Mi Kyung\} and Fraser, \{Paul J.\} and Hyeri Park and Sohyeon Geum and Jens M{\"u}hle and Jooil Kim and Ian Porter and Salameh, \{Peter K.\} and Harth, \{Christina M.\} and Dunse, \{Bronwyn L.\} and Krummel, \{Paul B.\} and Weiss, \{Ray F.\} and Simon O'Doherty and Dickon Young and Sunyoung Park",

note = "Funding Information: Financial support. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University. Funding Information: This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens M?hle, Christina M. Harth, Peter K. Salameh, and Ray F.Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University. Funding Information: Acknowledgements. This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens M{\"u}hle, Christina M. Harth, Peter K. Salameh, and Ray F. Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University. Publisher Copyright: {\textcopyright} 2022 Haklim Choi et al.",

year = "2022",

month = apr,

day = "20",

doi = "10.5194/acp-22-5157-2022",

language = "English",

volume = "22",

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journal = "Atmospheric Chemistry and Physics",

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Choi, H, Park, MK, Fraser, PJ, Park, H, Geum, S, Mühle, J, Kim, J, Porter, I, Salameh, PK, Harth, CM, Dunse, BL, Krummel, PB, Weiss, RF, O'Doherty, S, Young, D & Park, S 2022, 'Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China', Atmospheric Chemistry and Physics, vol. 22, no. 8, pp. 5157-5173. https://doi.org/10.5194/acp-22-5157-2022

TY - JOUR

T1 - Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China

AU - Choi, Haklim

AU - Park, Mi Kyung

AU - Fraser, Paul J.

AU - Park, Hyeri

AU - Geum, Sohyeon

AU - Mühle, Jens

AU - Kim, Jooil

AU - Porter, Ian

AU - Salameh, Peter K.

AU - Harth, Christina M.

AU - Dunse, Bronwyn L.

AU - Krummel, Paul B.

AU - Weiss, Ray F.

AU - O'Doherty, Simon

AU - Young, Dickon

AU - Park, Sunyoung

N1 - Funding Information: Financial support. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University. Funding Information: This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens M?hle, Christina M. Harth, Peter K. Salameh, and Ray F.Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University. This research has been supported by the National Research Foundation of Korea (grant no. 2020R1A2C3003774), National Aeronautics and Space Administration (grant nos. NNX16AC96G, NNX16AC97G, and NNX16AC98G), the Australian Bureau of Meteorology, CSIRO, the Australian Department of Agriculture, Water and the Environment, and La Trobe University. Funding Information: Acknowledgements. This research was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT). Support for contributions by Jooil Kim, Jens Mühle, Christina M. Harth, Peter K. Salameh, and Ray F. Weiss came from National Aeronautics and Space Administration. Support for contributions by Paul J. Fraser, Bronwyn L Dunse, and Paul B. Krummel came from National Aeronautics and Space Administration, the Australian Bureau of Meteorology, CSIRO, and the Australian Department of Agriculture, Water and the Environment (DAWE). Support for contributions by Ian Porter was provided by La Trobe University. Publisher Copyright: © 2022 Haklim Choi et al.

PY - 2022/4/20

Y1 - 2022/4/20

N2 - Methyl bromide (CH3Br) is a potent ozone-depleting substance (ODS) that has both natural and anthropogenic sources. CH3Br has been used mainly for preplant soil fumigation, post-harvest grain and timber fumigation, and structural fumigation. Most non-quarantine and pre-shipment (non-QPS) uses were phased out by 2005 for non-Article 5 (developed) countries and by 2015 for Article 5 (developing) countries under the Montreal Protocol on Substances that Deplete the Ozone Layer; some uses have continued under critical-use exemptions (CUEs). Under the protocol, individual nations are required to report annual data on CH3Br production and consumption for quarantine-pre-shipment (QPS) uses, non-QPS uses, and CUEs to the United Nations Environment Programme (UNEP). In this study, we analyzed high-precision, in situ measurements of atmospheric mole fractions of CH3Br obtained at the Gosan station on Jeju Island, South Korea, from 2008 to 2019. The background mole fractions of CH3Br in the atmosphere at Gosan declined from 8.5±0.8gppt (parts per trillion) in 2008 to 7.4±0.6gppt in 2019 at a rate of -0.13±0.02gpptgyr-1. At Gosan, we also observed periods of persistent mole fractions (pollution events) elevated above the decreasing background in continental air masses from China. Statistical back-trajectory analyses showed that these pollution events are predominantly traced back to CH3Br emissions from eastern China. Using an interspecies correlation (ISC) method with the reference trace species CFC-11 (CCl3F), we estimate anthropogenic CH3Br emissions from eastern China at an average of 4.1±1.3gGggyr-1 in 2008-2019, approximately 2.9±1.3gGggyr-1 higher than the bottom-up emission estimates reported to UNEP. Possible non-fumigation CH3Br sources - rapeseed production and biomass burning - were assessed, and it was found that the discrepancy is most likely due to unreported or incorrectly reported QPS and non-QPS fumigation uses. These unreported anthropogenic emissions of CH3Br are confined to eastern China and account for 30g%-40g% of anthropogenic global CH3Br emissions. They are likely due to delays in the introduction of CH3Br alternatives, such as sulfuryl fluoride (SO2F2), heat, and irradiation, and a possible lack of industry awareness of the need for regulation of CH3Br production and use.

AB - Methyl bromide (CH3Br) is a potent ozone-depleting substance (ODS) that has both natural and anthropogenic sources. CH3Br has been used mainly for preplant soil fumigation, post-harvest grain and timber fumigation, and structural fumigation. Most non-quarantine and pre-shipment (non-QPS) uses were phased out by 2005 for non-Article 5 (developed) countries and by 2015 for Article 5 (developing) countries under the Montreal Protocol on Substances that Deplete the Ozone Layer; some uses have continued under critical-use exemptions (CUEs). Under the protocol, individual nations are required to report annual data on CH3Br production and consumption for quarantine-pre-shipment (QPS) uses, non-QPS uses, and CUEs to the United Nations Environment Programme (UNEP). In this study, we analyzed high-precision, in situ measurements of atmospheric mole fractions of CH3Br obtained at the Gosan station on Jeju Island, South Korea, from 2008 to 2019. The background mole fractions of CH3Br in the atmosphere at Gosan declined from 8.5±0.8gppt (parts per trillion) in 2008 to 7.4±0.6gppt in 2019 at a rate of -0.13±0.02gpptgyr-1. At Gosan, we also observed periods of persistent mole fractions (pollution events) elevated above the decreasing background in continental air masses from China. Statistical back-trajectory analyses showed that these pollution events are predominantly traced back to CH3Br emissions from eastern China. Using an interspecies correlation (ISC) method with the reference trace species CFC-11 (CCl3F), we estimate anthropogenic CH3Br emissions from eastern China at an average of 4.1±1.3gGggyr-1 in 2008-2019, approximately 2.9±1.3gGggyr-1 higher than the bottom-up emission estimates reported to UNEP. Possible non-fumigation CH3Br sources - rapeseed production and biomass burning - were assessed, and it was found that the discrepancy is most likely due to unreported or incorrectly reported QPS and non-QPS fumigation uses. These unreported anthropogenic emissions of CH3Br are confined to eastern China and account for 30g%-40g% of anthropogenic global CH3Br emissions. They are likely due to delays in the introduction of CH3Br alternatives, such as sulfuryl fluoride (SO2F2), heat, and irradiation, and a possible lack of industry awareness of the need for regulation of CH3Br production and use.

UR - https://www.scopus.com/pages/publications/85129283780

U2 - 10.5194/acp-22-5157-2022

DO - 10.5194/acp-22-5157-2022

M3 - Article (Academic Journal)

AN - SCOPUS:85129283780

SN - 1680-7316

VL - 22

SP - 5157

EP - 5173

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 8

ER -

Top-down and bottom-up estimates of anthropogenic methyl bromide emissions from eastern China

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