Abstract
The early detection of a global emission increase of CFC-11 after 2012 (Montzka et al., 2018) alerted society to a possible violation of the Montreal Protocol on Substances that Deplete the Ozone Layer (MP). This early alert resulted in parties participating in the MP taking urgent actions (United Nations Environment Programme (UNEP), 2019). As a result, atmospheric measurements made in 2019 suggest a sharp decline in global CFC-11 emissions (Montzka et al., 2021). Despite the success in the early detection and mitigation of some of this problem, regions fully responsible for the recent global emission changes of CFC-11 have not yet been identified. Roughly two thirds (60 ± 40 %) of the emission increase between 2008–2012 and 2014–2017 and two thirds (60 ± 30 %) of emission decline between 2014–2017 and 2019 was explained by regional emission changes in eastern mainland China (Park et al., 2021; Rigby et al., 2019). Here, we used atmospheric CFC-11 measurements made from two global aircraft surveys, the HIAPER Pole-to-Pole Observations (HIPPO) in November 2009–September 2011 and the Atmospheric Tomography Mission (ATom) in August 2016–May 2018, in combination with the global CFC-11 measurements made by the U.S. National Oceanic and Atmospheric Administration during these two periods, to derive global and regional emission changes of CFC-11. Our results suggest Asia accounted for the largest fractions of global CFC-11 emissions in both periods, 43 (37–52) % during November 2009–September 2011 and 57 (49–62) % during August 2016–May 2018. Asia was also primarily responsible for the emission increase between these two periods, accounting for 86 (59–115) % of the global CFC-11 emission rise between the two periods. Besides eastern mainland China, we find that temperate western Asia and tropical Asia also contributed significantly to global CFC-11 emissions during both periods and likely to the global CFC-11 emission increase between these periods. Besides Asia, the atmospheric observations also provide strong constraints on CFC-11 emissions from North America and Europe, suggesting that each of them accounted for 10–15 % of global CFC-11 emissions during the HIPPO period and smaller fractions in the ATom period. For South America, Africa, and Australia, the derived regional emissions had larger dependence on the prior assumptions of emissions and emission changes, due to a lower sensitivity of the observations considered here to emissions from these regions. However, significant increases in CFC-11 emissions from the southern hemispheric lands were not likely due to the observed increase of north-to-south interhemispheric gradients in atmospheric CFC-11 mole fractions from 2012 to 2017.
Highlights
Trichlorofluoromethane, CFC-11, is a potent ozone depleting substance, whose production has been controlled by the Montreal Protocol since 1987
Increase of CFC-11 emissions between the HIAPER Pole-toPole Observations (HIPPO) and Atmospheric Tomography (ATom) periods observed in remote atmospheric observations
Earth’s surface, a similar magnitude of this slow-down in atmospheric CFC-11 mole fraction decline is apparent throughout the free troposphere in the aircraft profiles obtained during the HIPPO and ATom campaigns (Fig. 4)
Summary
Trichlorofluoromethane, CFC-11, is a potent ozone depleting substance, whose production has been controlled by the Montreal Protocol since 1987. Despite the international effort to understand the origin of this large global emission increase of CFC-11, only a portion of the emission rise (60 ± 40 %) could be explained by emission increases from eastern mainland China (Rigby et al, 2019; Adcock et al, 2020; Park et al, 2021). It remains unclear where the rest of the global CFC-11 emission increase originated
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