ALBERT

Description: Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget,

Description: 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.

Description: We report continuous surface observations of carbon dioxide (CO2) and methane (CH4) from the Los Angeles (LA) Megacity Carbon Project during 2015. We devised a calibration strategy, methods for selection of background air masses, calculation of urban enhancements, and a detailed algorithm for estimating uncertainties in urban-scale CO2 and CH4 measurements. These methods are essential for understanding carbon fluxes from the LA megacity and other complex urban environments globally. We estimate background mole fractions entering LA using observations from four extra-urban sites including two marine sites located south of LA in La Jolla (LJO) and offshore on San Clemente Island (SCI), one continental site located in Victorville (VIC), in the high desert northeast of LA, and one continental/mid-troposphere site located on Mount Wilson (MWO) in the San Gabriel Mountains. We find that a local marine background can be established to within  ∼  1 ppm CO2 and  ∼  10 ppb CH4 using these local measurement sites. Overall, atmospheric carbon dioxide and methane levels are highly variable across Los Angeles. Urban and suburban sites show moderate to large CO2 and CH4 enhancements relative to a marine background estimate. The USC (University of Southern California) site near downtown LA exhibits median hourly enhancements of  ∼  20 ppm CO2 and  ∼  150 ppb CH4 during 2015 as well as  ∼  15 ppm CO2 and  ∼  80 ppb CH4 during mid-afternoon hours (12:00–16:00 LT, local time), which is the typical period of focus for flux inversions. The estimated measurement uncertainty is typically better than 0.1 ppm CO2 and 1 ppb CH4 based on the repeated standard gas measurements from the LA sites during the last 2 years, similar to Andrews et al. (2014). The largest component of the measurement uncertainty is due to the single-point calibration method; however, the uncertainty in the background mole fraction is much larger than the measurement uncertainty. The background uncertainty for the marine background estimate is  ∼  10 and  ∼  15 % of the median mid-afternoon enhancement near downtown LA for CO2 and CH4, respectively. Overall, analytical and background uncertainties are small relative to the local CO2 and CH4 enhancements; however, our results suggest that reducing the uncertainty to less than 5 % of the median mid-afternoon enhancement will require detailed assessment of the impact of meteorology on background conditions.

Description: In a changing climate, potential stratospheric circulation changes require long-term monitoring. Stratospheric trace gas measurements are often used as a proxy for stratospheric circulation changes via the mean age of air values derived from them. In this study, we investigated five potential age of air tracers – the perfluorocarbons CF4, C2F6 and C3F8 and the hydrofluorocarbons CHF3 (HFC-23) and HFC-125 – and compare them to the traditional tracer SF6 and a (relatively) shorter-lived species, HFC-227ea. A detailed uncertainty analysis was performed on mean ages derived from these new tracers to allow us to confidently compare their efficacy as age tracers to the existing tracer, SF6. Our results showed that uncertainties associated with the mean age derived from these new age tracers are similar to those derived from SF6, suggesting that these alternative compounds are suitable in this respect for use as age tracers. Independent verification of the suitability of these age tracers is provided by a comparison between samples analysed at the University of East Anglia and the Scripps Institution of Oceanography. All five tracers give younger mean ages than SF6, a discrepancy that increases with increasing mean age. Our findings qualitatively support recent work that suggests that the stratospheric lifetime of SF6 is significantly less than the previous estimate of 3200 years. The impact of these younger mean ages on three policy-relevant parameters – stratospheric lifetimes, fractional release factors (FRFs) and ozone depletion potentials – is investigated in combination with a recently improved methodology to calculate FRFs. Updates to previous estimations for these parameters are provided.

Description: High frequency measurements of trifluoromethane (HFC-23, CHF3), a potent hydrofluorocarbon greenhouse gas, largely emitted to the atmosphere as a by-product of the production of the hydrochlorofluorocarbon HCFC-22 (CHClF2), at five core stations of the Advanced Global Atmospheric Gases Experiment (AGAGE) network, combined with measurements on firn air, old Northern Hemisphere air samples and Cape Grim Air Archive (CGAA) air samples, are used to explore the current and historic changes in the atmospheric abundance of HFC-23. These measurements are used in combination with the AGAGE 2-D atmospheric 12-box model and a Bayesian inversion methodology to determine model atmospheric mole fractions and the history of global HFC-23 emissions. The global modelled annual mole fraction of HFC-23 in the background atmosphere was 28.9 ± 0.6 pmol mol−1 at the end of 2016, representing a 28 % increase from 22.6 ± 0.4 pmol mol−1 in 2009. Over the same time frame, the modelled mole fraction of HCFC-22 increased by 19 % from 199 ± 2 to 237 ± 2 pmol mol−1. However, unlike HFC-23, the annual average HCFC-22 growth rate slowed from 2009 to 2016 at an annual average rate of −0.5 pmol mol−1 yr−2. This slowing atmospheric growth is consistent with HCFC-22 moving from dispersive (high fractional emissions) to feedstock (low fractional emissions) uses, with HFC-23 emissions remaining as a consequence of incomplete mitigation from all HCFC-22 production.Our results demonstrate that, following a minimum in HFC-23 global emissions in 2009 of 9.6 ± 0.6, emissions increased to a maximum in 2014 of 14.5 ± 0.6 Gg yr−1 and then declined to 12.7 ± 0.6 Gg yr−1 (157 Mt CO2 eq. yr−1) in 2016. The 2009 emissions minimum is consistent with estimates based on national reports and is likely a response to the implementation of the Clean Development Mechanism (CDM) to mitigate HFC-23 emissions by incineration in developing (non-Annex 1) countries under the Kyoto Protocol. Our derived cumulative emissions of HFC-23 during 2010–2016 were 89 ± 2 Gg (1.1 ± 0.2 Gt CO2 eq.), which led to an increase in radiative forcing of 1.0 ± 0.1 mW m−2 over the same period. Although the CDM had reduced global HFC-23 emissions, it cannot now offset the higher emissions from increasing HCFC-22 production in non-Annex 1 countries, as the CDM was closed to new entrants in 2009. We also find that the cumulative European HFC-23 emissions from 2010 to 2016 were  ∼  1.3 Gg, corresponding to just 1.5 % of cumulative global HFC-23 emissions over this same period. The majority of the increase in global HFC-23 emissions since 2010 is attributed to a delay in the adoption of mitigation technologies, predominantly in China and East Asia. However, a reduction in emissions is anticipated, when the Kigali 2016 amendment to the Montreal Protocol, requiring HCFC and HFC production facilities to introduce destruction of HFC-23, is fully implemented.

Description: Decadal trends in the atmospheric abundances of carbon tetrafluoride (CF4) and nitrogen trifluoride (NF3) have been well characterised and have provided a time series of global total emissions. Information on locations of emissions contributing to the global total, however, is currently poor. We use a unique set of measurements between 2008 and 2015 from the Gosan station, Jeju Island, South Korea (part of the Advanced Global Atmospheric Gases Experiment network), together with an atmospheric transport model, to make spatially disaggregated emission estimates of these gases in East Asia. Due to the poor availability of good prior information for this study, our emission estimates are largely influenced by the atmospheric measurements. Notably, we are able to highlight emission hotspots of NF3 and CF4 in South Korea due to the measurement location. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.3±2.7 and 0.36±0.11 Gg yr−1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6±0.07 Gg yr−1 in 2015, which equates to ∼1.6 % of the country's CO2 emissions. We also apply our method to calculate emissions of CHF3 (HFC-23) between 2008 and 2012, for which our results find good agreement with other studies and which helps support our choice in methodology for CF4 and NF3.

Description: We present top-down constraints on global monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies include (1) a standard 4D-Var inversion at native model resolution (4° × 5°), (2) an inversion for six continental and three ocean regions, and (3) a fast 4D-Var inversion based on a novel dimension reduction technique employing randomized singular value decomposition (SVD). The optimized global flux ranges from 15.9 Tg N yr−1 (SVD-based inversion) to 17.5–17.7 Tg N yr−1 (continental-scale, standard 4D-Var inversions), with the former better capturing the extratropical N2O background measured during the HIAPER Pole-to-Pole Observations (HIPPO) airborne campaigns. We find that the tropics provide a greater contribution to the global N2O flux than is predicted by the prior bottom-up inventories, likely due to underestimated agricultural and oceanic emissions. We infer an overestimate of natural soil emissions in the extratropics and find that predicted emissions are seasonally biased in northern midlatitudes. Here, optimized fluxes exhibit a springtime peak consistent with the timing of spring fertilizer and manure application, soil thawing, and elevated soil moisture. Finally, the inversions reveal a major emission underestimate in the US Corn Belt in the bottom-up inventory used here. We extensively test the impact of initial conditions on the analysis and recommend formally optimizing the initial N2O distribution to avoid biasing the inferred fluxes. We find that the SVD-based approach provides a powerful framework for deriving emission information from N2O observations: by defining the optimal resolution of the solution based on the information content of the inversion, it provides spatial information that is lost when aggregating to political or geographic regions, while also providing more temporal information than a standard 4D-Var inversion.

Description: Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), ΣCFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry-air mole fraction in parts per trillion, pmol mol−1) in 2016. Its growth rate has decreased since the mid-1980s but has remained at a surprisingly high mean level of 0.02 ppt yr−1 since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. ΣCFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.49 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unchanging lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (〉 15 % of past peak emissions), of ΣCFC-114 at 1.90 ± 0.84 kt yr−1 (∼ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (〉 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2015–2016 are 1.14 ± 0.50 kt yr−1 and have doubled compared to the 2007–2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012–2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for ΣCFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.

Description: High-frequency, in situ global observations of HCFC-22 (CHClF2), HCFC-141b (CH3CCl2F), HCFC-142b (CH3CClF2) and HCFC-124 (CHClFCF3) and their main HFC replacements, HFC-134a (CH2FCF3), HFC-125 (CHF2CF3), HFC-143a (CH3CF3) and HFC-32 (CH2F2), have been used to determine their changing global growth rates and emissions in response to the Montreal Protocol and its recent amendments. Global mean mole fractions of HCFC-22, -141b, and -142b have increased throughout the observation period, reaching 234, 24.3 and 22.4 pmol mol−1, respectively, in 2015. HCFC-124 reached a maximum global mean mole fraction of 1.48 pmol mol−1 in 2007 and has since declined by 23 % to 1.14 pmol mol−1 in 2015. The HFCs all show increasing global mean mole fractions. In 2015 the global mean mole fractions (pmol mol−1) were 83.3 (HFC-134a), 18.4 (HFC-125), 17.7 (HFC-143a) and 10.5 (HFC-32). The 2007 adjustment to the Montreal Protocol required the accelerated phase-out of emissive uses of HCFCs with global production and consumption capped in 2013 to mitigate their environmental impact as both ozone-depleting substances and important greenhouse gases. We find that this change has coincided with a stabilisation, or moderate reduction, in global emissions of the four HCFCs with aggregated global emissions in 2015 of 449 ± 75 Gg yr−1, in CO2 equivalent units (CO2 eq.) 0.76 ± 0.1 Gt yr−1, compared with 483 ± 70 Gg yr−1 (0.82 ± 0.1 Gt yr−1 CO2 eq.) in 2010 (uncertainties are 1σ throughout this paper). About 79 % of the total HCFC atmospheric burden in 2015 is HCFC-22, where global emissions appear to have been relatively similar since 2011, in spite of the 2013 cap on emissive uses. We attribute this to a probable increase in production and consumption of HCFC-22 in Montreal Protocol Article 5 (developing) countries and the continuing release of HCFC-22 from the large banks which dominate HCFC global emissions. Conversely, the four HFCs all show increasing mole fraction growth rates with aggregated global HFC emissions of 327 ± 70 Gg yr−1 (0.65 ± 0.12 Gt yr−1 CO2 eq.) in 2015 compared to 240 ± 50 Gg yr−1 (0.47 ± 0.08 Gt yr−1 CO2 eq.) in 2010. We also note that emissions of HFC-125 and HFC-32 appear to have increased more rapidly averaged over the 5-year period 2011–2015, compared to 2006–2010. As noted by Lunt et al. (2015) this may reflect a change to refrigerant blends, such as R-410A, which contain HFC-32 and -125 as a 50 : 50 blend.

Description: Carbon tetrachloride (CCl4) is a first-generation ozone-depleting substance, and its emissive use and production were globally banned by the Montreal Protocol with a 2010 phase-out; however, production and consumption for non-dispersive use as a chemical feedstock and as a process agent are still allowed. This study uses the high frequency and magnitude of CCl4 pollution events from an 8-year real-time atmospheric measurement record obtained at Gosan station (a regional background monitoring site in East Asia) to present evidence of significant unreported emissions of CCl4. Top-down emissions of CCl4 amounting to 23.6±7.1 Gg yr−1 from 2011 to 2015 are estimated for China, in contrast to the most recently reported, post-2010, Chinese bottom-up emissions of 4.3–5.2 Gg yr−1. The missing emissions (∼19 Gg yr−1) for China contribute to approximately 54 % of global CCl4 emissions. It is also shown that 89 %±6 % of CCl4 enhancements observed at Gosan are related to CCl4 emissions from the production of CH3Cl, CH2Cl2, CHCl3 and C2Cl4 and its usage as a feedstock and process agent in chemical manufacturing industries. Specific sources and processes are identified using statistical methods, and it is considered highly unlikely that CCl4 is emitted by dispersive uses such as old landfills, contaminated soils and solvent usage. It is thus crucial to implement technical improvements and better regulation strategies to reduce evaporative losses of CCl4 occurring at the factory and/or process levels.