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±0.8 ppt (parts per trillion) in 2008 to 7.4±0.6 ppt in 2019 at a rate of -0.13±0.02 ppt yr−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±1.3 Gg yr−1 in 2008–2019, approximately 2.9±1.3 Gg yr−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 30 %–40 % 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.