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National greenhouse gas inventories (GHGIs) are submitted annually to the United Nations Framework Convention on Climate Change (UNFCCC). They are estimated in compliance with Intergovernmental Panel on Climate Change (IPCC) methodological guidance using activity data, emission factors and facility-level measurements. For some sources, the outputs from these calculations are very uncertain. Inverse modelling techniques that use high-quality, long-term measurements of atmospheric gases have been developed to provide independent verification of national GHGIs. This is considered good practice by the IPCC as it helps national inventory compilers to verify reported emissions and to reduce emission uncertainty. Emission estimates from the InTEM (Inversion Technique for Emission Modelling) model are presented for the UK for the hydrofluorocarbons (HFCs) reported to the UNFCCC (HFC-125, HFC-134a, HFC-143a, HFC-152a, HFC-23, HFC-32, HFC-227ea, HFC-245fa, HFC-43-10mee and HFC-365mfc). These HFCs have high global warming potentials (GWPs), and the global background mole fractions of all but two are increasing, thus highlighting their relevance to the climate and a need for increasing the accuracy of emission estimation for regulatory purposes. This study presents evidence that the long-term annual increase in growth of HFC-134a has stopped and is now decreasing. For HFC-32 there is an early indication, its rapid global growth period has ended, and there is evidence that the annual increase in global growth for HFC-125 has slowed from 2018. The inverse modelling results indicate that the UK implementation of European Union regulation of HFC emissions has been successful in initiating a decline in UK emissions from 2018. Comparison of the total InTEM UK HFC emissions in 2020 with the average from 2009–2012 shows a drop of 35 %, indicating progress toward the target of a 79 % decrease in sales by 2030. The total InTEM HFC emission estimates (2008–2018) are on average 73 (62–83) % of, or 4.3 (2.7–5.9) Tg CO2-eq yr−1 lower than, the total HFC emission estimates from the UK GHGI. There are also significant discrepancies between the two estimates for the individual HFCs.

We present a method for estimating fossil fuel methane emissions using observations of methane and ethane, accounting for uncertainty in their emission ratio. The ethane:methane emission ratio is incorporated as a spatially and temporally variable parameter in a Bayesian model, with its own prior distribution and uncertainty. We find that using an emission ratio distribution mitigates bias from using a fixed, potentially incorrect emission ratio and that uncertainty in this ratio is propagated into posterior estimates of emissions. A synthetic data test is used to show the impact of assuming an incorrect ethane:methane emission ratio and demonstrate how our variable parameter model can better quantify overall uncertainty. We also use this method to estimate UK methane emissions from high-frequency observations of methane and ethane from the UK Deriving Emissions linked to Climate Change (DECC) network. Using the joint methane–ethane inverse model, we estimate annual mean UK methane emissions of approximately 0.27 (95 % uncertainty interval 0.26–0.29) Tg yr−1 from fossil fuel sources and 2.06 (1.99–2.15) Tg yr−1 from non-fossil fuel sources, during the period 2015–2019. Uncertainties in UK fossil fuel emissions estimates are reduced on average by 15 % and up to 35 % when incorporating ethane into the inverse model, in comparison to results from the methane-only inversion.

We reconstruct atmospheric abundances of the potent greenhouse gas c - C4F8 (perfluorocyclobutane, perfluorocarbon PFC-318) from measurements of in situ, archived, firn, and aircraft air samples with precisions of ∼1 %–2 % reported on the SIO-14 gravimetric calibration scale. Combined with inverse methods, we found near-zero atmospheric abundances from the early 1900s to the early 1960s, after which they rose sharply, reaching 1.66 ppt (parts per trillion dry-air mole fraction) in 2017. Global c - C4F8 emissions rose from near zero in the 1960s to 1.2±0.1 (1 σ ) Gg yr −1 in the late 1970s to late 1980s, then declined to 0.77±0.03 Gg yr −1 in the mid-1990s to early 2000s, followed by a rise since the early 2000s to 2.20±0.05 Gg yr −1 in 2017. These emissions are significantly larger than inventory-based emission estimates. Estimated emissions from eastern Asia rose from 0.36 Gg yr −1 in 2010 to 0.73 Gg yr −1 in 2016 and 2017, 31 % of global emissions, mostly from eastern China. We estimate emissions of 0.14 Gg yr −1 from northern and central India in 2016 and find evidence for significant emissions from Russia. In contrast, recent emissions from northwestern Europe and Australia are estimated to be small ( ≤1 % each). We suggest that emissions from China, India, and Russia are likely related to production of polytetrafluoroethylene (PTFE, “Teflon”) and other fluoropolymers and fluorochemicals that are based on the pyrolysis of hydrochlorofluorocarbon HCFC-22 ( CHClF2 ) in which c - C4F8 is a known by-product. The semiconductor sector, where c - C4F8 is used, is estimated to be a small source, at least in South Korea, Japan, Taiwan, and Europe. Without an obvious correlation with population density, incineration of waste-containing fluoropolymers is probably a minor source, and we find no evidence of emissions from electrolytic production of aluminum in Australia. While many possible emissive uses of c - C4F8 are known and though we cannot categorically exclude unknown sources, the start of significant emissions may well be related to the advent of commercial PTFE production in 1947. Process controls or abatement to reduce the c - C4F8 by-product were probably not in place in the early decades, explaining the increase in emissions in the 1960s and 1970s. With the advent of by-product reporting requirements to the United Nations Framework Convention on Climate Change (UNFCCC) in the 1990s, concern about climate change and product stewardship, abatement, and perhaps the collection of c - C4F8 by-product for use in the semiconductor industry where it can be easily abated, it is conceivable that emissions in developed countries were stabilized and then reduced, explaining the observed emission reduction in the 1980s and 1990s. Concurrently, production of PTFE in China began to increase rapidly. Without emission reduction requirements, it is plausible that global emissions today are dominated by China and other developing countries. We predict that c - C4F8 emissions will continue to rise and that c - C4F8 will become the second most important emitted PFC in terms of CO2 -equivalent emissions within a year or two. The 2017 radiative forcing of c - C4F8 (0.52 mW m −2 ) is small but emissions of c - C4F8 and other PFCs, due to their very long atmospheric lifetimes, essentially permanently alter Earth's radiative budget and should be reduced. Significant emissions inferred outside of the investigated regions clearly show that observational capabilities and reporting requirements need to be improved to understand global and country-scale emissions of PFCs and other synthetic greenhouse gases and ozone-depleting substances.

Under the Kigali Amendment to the Montreal Protocol, new controls are being implemented to reduce emissions of HFC-23 (CHF\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{3}$$\end{document}3), a by-product during the manufacture of HCFC-22 (CHClF\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{2}$$\end{document}2). Starting in 2015, China and India, who dominate global HCFC-22 production (75% in 2017), set out ambitious programs to reduce HFC-23 emissions. Here, we estimate that these measures should have seen global emissions drop by 87% between 2014 and 2017. Instead, atmospheric observations show that emissions have increased and in 2018 were higher than at any point in history (15.9 \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\pm \ 0.9\ {\rm{{Gg}}\ {{{yr}}}^{-1}}$$\end{document}±0.9Ggyr−1). Given the magnitude of the discrepancy between expected and observation-inferred emissions, it is likely that the reported reductions have not fully materialized or there may be substantial unreported production of HCFC-22, resulting in unaccounted-for HFC-23 by-product emissions. The difference between reported and observation-inferred estimates suggests that an additional ~309 Tg \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${{\rm{CO}}}_{2}$$\end{document}CO2-equivalent emissions were added to the atmosphere between 2015 and 2017., International agreements have been implemented to reduce emissions of hydrofluorocarbons (HFCs) to reduce their radiative forcing. Even though reported HFC-23 emissions are at a historical low, observations indicate that emissions have actually increased over recent years to higher levels than previously.

Methane is a strong contributor to global climate change, yet our current understanding and quantification of its sources and their variability is incomplete. There is a growing need for comparisons between emission estimates produced using bottom-up inventory approaches and top-down inversion techniques based on atmospheric measurements, especially at higher spatial resolutions. To meet this need, this study presents using an inversion approach based on the Inversion Technique for Emissions Modelling (InTEM) framework and measurements from four sites in East Anglia, United Kingdom. Atmospheric methane concentrations were recorded at 1–2 minute time-steps at each location within the region of interest. These observations, coupled with the UK Met Office's Lagrangian particle dispersion model, NAME (Numerical Atmospheric dispersion Modelling Environment), were used within InTEM2014 to produce methane emission estimates for a 1-year period (June 2013–May 2014) in this eastern region of the UK (~ 100 × 150 km) at high spatial resolution (up to 4 × 4 km). InTEM2014 was able to produce realistic emissions estimates for East Anglia, and highlighted potential areas of difference from the UK National Atmospheric Emissions Inventory (NAEI). As this study was part of the UK Greenhouse gAs Uk and Global Emissions (GAUGE) project, observations were included within a national inversion using all eleven measurement sites across the UK to directly compare emission estimates for the East Anglia Region. Results show similar methane estimates for the East Anglia region. Methane emissions from Norfolk and Suffolk show good agreement with the estimates in NAEI, with differences of ~ 5 %. Larger differences are found for Cambridgeshire where our estimate is 22.5 % lower than that of NAEI. The addition of the EA sites within the national inversion system enabled finer spatial resolution and a decrease in the associated uncertainty for that area. Further development of our approach to include a more robust analysis of the methane concentration in the air entering this region and the uncertainty associated with the resulting emissions would strengthen this inverse method. Nonetheless, our results show there is value in high spatial resolution measurement networks and the resulting inversion emission estimates.