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Abstract. Production and consumption of CFC-11 (trichlorofluoromethane, CCl3F), CFC-12 (dichlorodifluoromethane, CCl2F2) and CCl4 (carbon tetrachloride) are controlled under the regulations of the Montreal Protocol and have been phased out globally since 2010. Only CCl4 is still widely produced as a chemical feedstock. After 2010, emissions of CFC-11 and CFC-12 should therefore mostly originate from existing banks (e.g. from foams, mobile air conditioning units and refrigerators); however evidence has emerged of an increase in global emissions of CFC-11 in the last decade, some of which has not been fully accounted for. The motivation for this work was to assess the emissions of CFC-11, CFC-12 and CCl4 from western Europe. All countries in this region have been subject to the controls of the Montreal Protocol since the late 1980s and, as non-Article 5 Parties, have been prohibited from producing CFCs and CCl4 for dispersive use since 1996. Four different inverse modelling systems are used to estimate emissions of these gases from 2008 to 2021 using data from four atmospheric measurement stations: Mace Head (Ireland), Jungfraujoch (Switzerland), Monte Cimone (Italy) and Tacolneston (UK). The average of the four model studies found that western European emissions of CFC-11, CFC-12 and CCl4 between 2008 and 2021 were declining at 3.5 % yr−1 (2.7 % yr−1–4.8 % yr−1), 7.7 % yr−1 (6.3 % yr−1–8.0 % yr−1) and 4.4 % yr−1 (2.6 % yr−1–6.4 % yr−1), respectively. Even though the emissions were declining throughout the period, the area including northern France, Belgium, the Netherlands and Luxembourg showed consistently elevated emissions of CFC-11 compared with the surrounding regions. Emissions of CFC-12 were slightly elevated in the same region. CCl4 emissions were the highest in the south of France. France had the highest emissions of all three gases over the period 2008–2021. Emissions from western Europe (2008–2021) were on average 2.4 ± 0.4 Gg (CFC-11), 1.3 ± 0.3 Gg (CFC-12) and 0.9 ± 0.2 Gg (CCl4). Our estimated decline in emissions of CFC-11 is consistent with a western European bank release rate of 3.4 % (2.6 %–4.5 %). This study concludes that emissions of CFC-11, CFC-12 and CCl4 have all declined from 2008 to 2021 in western Europe. Therefore, no evidence is found that western European emissions contributed to the unexplained part of the global increase in atmospheric concentrations of CFC-11 observed in the last decade.

To mitigate the impact of greenhouse gas (GHG) and air pollutant emissions, it is of utmost importance to understand where emissions occur. In the real world, atmospheric pollutants are produced by various human activities from point sources (e.g. power plants and industrial facilities) but also from diffuse sources (e.g. residential activities and agriculture). However, as tracking all these single sources of emissions is practically impossible, emission inventories are typically compiled using national-level statistics by sector, which are then downscaled at the grid-cell level using spatial information. In this work, we develop high-spatial-resolution proxies for use in downscaling the national emission totals for all world countries provided by the Emissions Database for Global Atmospheric Research (EDGAR). In particular, in this paper, we present the latest EDGAR v8.0 GHG, which provides readily available emission data at different levels of spatial granularity, obtained from a consistently developed GHG emission database. This has been achieved through the improvement and development of high-resolution spatial proxies that allow for a more precise allocation of emissions over the globe. A key novelty of this work is the potential to analyse subnational GHG emissions over the European territory and also over the United States, China, India, and other high-emitting countries. These data not only meet the needs of atmospheric modellers but can also inform policymakers working in the field of climate change mitigation. For example, the EDGAR GHG emissions at the NUTS 2 level (Nomenclature of Territorial Units for Statistics level 2) over Europe contribute to the development of EU cohesion policies, identifying the progress of each region towards achieving the carbon neutrality target and providing insights into the highest-emitting sectors. The data can be accessed at 10.2905/b54d8149-2864-4fb9-96b9-5fd3a020c224 specifically for EDGAR v8.0 (Crippa et al., 2023a) and 10.2905/D67EEDA8-C03E-4421-95D0-0ADC460B9658 for the subnational dataset (Crippa et al., 2023b). [ABSTRACT FROM AUTHOR]

Knowing where emissions occur is essential for planning effective emission reduction measures and for atmospheric modelling. Emission inventories are typically compiled at national level and provide sector-specific emission estimates. Disaggregating national emissions on high-resolution grids requires spatial proxies that contain information on the location of different emission sources (e.g. point sources, linear and area sources). Knowing the correct allocation of emissions from point sources is essential to avoid the misallocating high emission levels. However, gathering information on point sources covering the entire globe and a wide temporal domain (1970 to present) is challenging due to limited data availability, accuracy of the reporting and completeness of data. The latest spatial proxies developed as part of the Emissions Database for Global Atmospheric Research (EDGARv8.0) provide the user with the possibility to work with different geographical details using a consistently developed GHG emissions database. A key novelty of EDGARv8.0 is the possibility to analyse sub-national GHG emissions over the European domain, but also over the US, China, India and main world countries. The relevance of using updated spatial information is assessed on the basis of regional case studies. [ABSTRACT FROM AUTHOR]

Production and consumption of CFC-11 (trichlorofluoromethane, CCl3F), CFC-12 dichlorodifluoromethane, CCl2F2) and CCl4 (carbon tetrachloride) are controlled under the regulations of the Montreal Protocol and have been phased out globally for dispersive use since 2010. Only CCl4 is still widely produced under exemption as a chemical feedstock (non-dispersive use). After 2010, emissions of CFC-11 and CFC-12 should therefore mostly originate from existing banks (e.g. foams and refrigerators), however evidence emerged of an increase in global emissions of CFC-11, which was in part attributed to eastern China. Emissions of CFC-11, CFC-12 and CCl4 have subsequently declined in this region, however the total global increase in CFC-11 was not fully accounted for. The motivation for this work was to assess the emissions of CFC-11 and the associated gases, CFC-12 and CCl4, from Western Europe. All countries in this region have been subject to the controls of the Montreal Protocol since the late 1980s, and, as non-Article-5 Parties, have been prohibited from producing CFCs and CCl4 for dispersive use since 1995. Four different inverse modelling systems are used to estimate emissions of these gases from 2008–2021 using data from four atmospheric measurement stations: Mace Head (Ireland), Jungfraujoch (Switzerland), Monte Cimone (Italy) and Tacolneston (UK). The average of the four model studies found that Western European emissions of CFC-11, CFC-12 and CCl4 between 2008 and 2021 were declining at 3.5 (2.7–4.8) %, 7.7 (6.3–8.0) % and 4.4 (2.6–6.4) % yr−1 respectively. Throughout this period, the highest CFC-11 emissions were in Northern France and Benelux (Belgium, the Netherlands and Luxembourg). Emissions of CFC-12 co-located in this region were slightly higher than elsewhere in Western Europe, and also showed some enhancement of CCl4 emissions. However for CCl4, emissions were highest in the south of France. France had the highest emissions of CFC-11, CFC-12 and CCl4 over the period 2008–2021. Emissions from Western Europe (2008–2021) were on average 2.4 ± 0.4 Gg (CFC-11), 1.3 ± 0.3 Gg (CFC-12), 0.9 ± 0.2 Gg (CCl4). This study concludes that the emissions of CFC-11 from Northern France and Benelux are unlikely to be the result of new production. Our estimated decline in emissions of CFC-11 is consistent with a Western European bank release rate of 3.4 (2.6–4.5) %, which is in the upper half of the published range. [ABSTRACT FROM AUTHOR]

We report a 40-year history of SF6 atmospheric mole fractions measured at the Advanced Global Atmospheric Gases Experiment (AGAGE) monitoring sites, combined with archived air samples, to determine emission estimates from 1978 to 2018. Previously we reported a global emission rate of 7.3±0.6 Gg yr-1 in 2008 and over the past decade emissions have continued to increase by about 24% to 9.04±0.35 Gg yr-1 in 2018. We show that changing patterns in SF6 consumption from developed (Kyoto Protocol Annex-1) to developing countries (non-Annex-1) and the rapid global expansion of the electric power industry, mainly in Asia, have increased the demand for SF6-insulated switchgear, circuit breakers, and transformers. The large bank of SF6 sequestered in this electrical equipment provides a substantial source of emissions from maintenance, replacement, and continuous leakage. Other emissive sources of SF6 occur from the magnesium, aluminium, and electronics industries as well as more minor industrial applications. More recently, reported emissions, including those from electrical equipment and metal industries, primarily in the Annex-1 countries, have declined steadily through substitution of alternative blanketing gases and technological improvements in less emissive equipment and more efficient industrial practices. Nevertheless, there are still demands for SF6 in Annex-1 countries due to economic growth, as well as continuing emissions from older equipment and additional emissions from newly installed SF6-insulated electrical equipment, although at low emission rates. In addition, in the non-Annex-1 countries, SF6 emissions have increased due to an expansion in the growth of the electrical power, metal, and electronics industries to support their continuing development. There is an annual difference of 2.5-5 Gg yr-1 (1990-2018) between our modelled top-down emissions and the UNFCCC-reported bottom-up emissions (United Nations Framework Convention on Climate Change), which we attempt to reconcile through analysis of the potential contribution of emissions from the various industrial applications which use SF6. We also investigate regional emissions in East Asia (China, S. Korea) and western Europe and their respective contributions to the global atmospheric SF6 inventory. On an average annual basis, our estimated emissions from the whole of China are approximately 10 times greater than emissions from western Europe. In 2018, our modelled Chinese and western European emissions accounted for ~ 36% and 3.1 %, respectively, of our global SF6 emissions estimate. [ABSTRACT FROM AUTHOR]

We report a 40-year history of SF6 atmospheric mole fractions measured at the Advanced Global Atmospheric Gases Experiment (AGAGE) monitoring sites, combined with archived air samples to determine emission estimates from 1978-2018. Previously we reported a global emission rate of 7.3 ± 0.6 Gigagrams (Gg) yr-1 in 2008 and over the past decade emissions have continued to increase by about 24 % to 9.04 ± 0.35 Gg yr-1 in 2018. We show that changing patterns in SF6 consumption from developed (Kyoto Protocol Annex-1) to developing countries (non-Annex-1) and the rapid global expansion of the electric power industry, mainly in Asia, have increased the demand for SF6-insulated switchgear, circuit breakers and transformers. The large bank of SF6 sequestered in this electrical equipment provides a substantial source of emissions from maintenance, replacement and continuous leakage. Other emissive sources of SF6 occur from the magnesium, aluminium, electronics industries and more minor industrial applications. More recently, reported emissions, including those from electrical equipment and metal industries, primarily in the Annex-1 countries, have steadily declined through substitution of alternative blanketing gases and technological improvements in less emissive equipment and more efficient industrial practices. Conversely, in the non-Annex-1 countries SF6 emissions have increased due to an expansion in the growth of the electrical power, metal and electronics industries to support their development. There is an annual difference of 2.5-5 Gg yr-1 (1990-2018) between our modelled top-down emissions and the UNFCCC reported bottom-up emissions, which we attempt to reconcile through analysis of the potential contribution of emissions from the various industrial applications which use SF6. We also investigate regional emissions in East Asia (China, S. Korea) and Western Europe and their respective contributions to the global atmospheric SF6 inventory. On an average annual basis, our estimated emissions from the whole of China are approximately 10 times greater than emissions from Western Europe. In 2018, our modelled Chinese and Western European emissions accounted for ~ 36 % and 3.1 %, respectively, of our global SF6 emissions estimate. [ABSTRACT FROM AUTHOR]

Carbon tetrachloride (CCl4) is a long-lived radiatively-active compound able to destroy stratospheric ozone. Due to its inclusion in the Montreal Protocol on Substances that Deplete the Ozone Layer, the last two decades have seen a sharp decrease in its large scale emissive use with a consequent decline of its atmospheric mole fractions. However, the Montreal Protocol restrictions do not apply to the use of carbon tetrachloride as feedstock for the production of other chemicals, implying the risk of fugitive emissions from the industry sector. The occurrence of such unintended emissions is suggested by a significant discrepancy between global emissions as derived by reported production and feedstock usage (bottom-up emissions), and those based on atmospheric observations (top-down emissions). In order to better constrain the atmospheric budget of carbon tetrachloride, several studies based on a combination of atmospheric observations and inverse modelling have been conducted in recent years in various regions of the world. This study is focused on the European scale and based on long-term high-frequency observations at three European sites, combined with a Bayesian inversion methodology. We estimated that average European emissions for 2006–2014 were 2.3 (± 0.8) Gg yr−1, with an average decreasing trend of 7.3 % per year. Our analysis identified France as the main source of emissions over the whole study period, with an average contribution to total European emissions of 25 %. The inversion was also able to allow the localisation of emission "hot-spots" in the domain, with major source areas in Southern France, Central England (UK) and Benelux (Belgium, The Netherlands, Luxembourg), where most of industrial scale production of basic organic chemicals are located. According to our results, European emissions correspond to 4.0 % of global emissions for 2006–2012. Together with other regional studies, our results allow a better constraint of the global budget of carbon tetrachloride and a better quantification of the gap between top-down and bottom-up estimates. [ABSTRACT FROM AUTHOR]