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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past 2 decades, primarily as a result of the phaseout of ozone-depleting substances under the Montreal Protocol and the use of HFCs as their replacements. In 2015, large increases were projected in HFC use and emissions in this century in the absence of regulations, contributing up to 0.5 ∘C to global surface warming by 2100. In 2019, the Kigali Amendment to the Montreal Protocol came into force with the goal of limiting the use of HFCs globally, and currently, regulations to limit the use of HFCs are in effect in several countries. Here, we analyze trends in HFC emissions inferred from observations of atmospheric abundances and compare them with previous projections. Total CO2 eq. inferred HFC emissions continue to increase through 2019 (to about 0.8 GtCO2eq.yr-1) but are about 20 % lower than previously projected for 2017–2019, mainly because of the lower global emissions of HFC-143a. This indicates that HFCs are used much less in industrial and commercial refrigeration (ICR) applications than previously projected. This is supported by data reported by the developed countries and the lower reported consumption of HFC-143a in China. Because this time period preceded the beginning of the Kigali provisions, this reduction cannot be linked directly to the provisions of the Kigali Amendment. However, it could indicate that companies transitioned away from the HFC-143a with its high global warming potential (GWP) for ICR applications in anticipation of national or global mandates. There are two new HFC scenarios developed based (1) on current trends in HFC use and Kigali-independent (K-I) control policies currently existing in several countries and (2) current HFC trends and compliance with the Kigali Amendment (KA-2022). These current policies reduce projected emissions in 2050 from the previously calculated 4.0–5.3 GtCO2eq.yr-1 to 1.9–3.6 GtCO2eq.yr-1. The added provisions of the Kigali Amendment are projected to reduce the emissions further to 0.9–1.0 GtCO2eq.yr-1 in 2050. Without any controls, projections suggest a HFC contribution of 0.28–0.44 ∘C to global surface warming by 2100, compared to a temperature contribution of 0.14–0.31 ∘C that is projected considering the national K-I policies current in place. Warming from HFCs is additionally limited by the Kigali Amendment controls to a contribution of about 0.04 ∘C by 2100.

In situ carbonyl sulfide (OCS) measurements from the Stratospheric Aerosol processes, Budget and Radiative Effects (SABRE) 2023 airborne campaign are used to evaluate the sulfate budget in the Arctic stratosphere during boreal winter. The strong correspondence between these measurements and remote retrievals from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer provide robust validation of the satellite's capability to monitor stratospheric OCS globally. We demonstrate how trends in the tropical tropopause layer and National Oceanic and Atmospheric Administration OCS surface data reveal a post‐2016 ∼8% global decline in OCS abundance, which is absent from many global climate models. New simulations with a revised planetary boundary layer OCS abundance show improved agreement with remote retrievals and in situ data across multiple stratospheric layers, but remaining model biases highlight the need for additional in situ OCS observations. The revised representation reduces the stratospheric sulfate burden, resulting in an increased shortwave solar flux at the tropical tropopause by as much as 0.3 Wm−2 locally, with implications for stratospheric circulation, radiative forcing, and climate feedbacks.

Sulfuryl fluoride (SO 2 F 2 ) is a synthetic pesticide and a potent greenhouse gas that is accumulating in the global atmosphere. Rising emissions are a concern since SO 2 F 2 has a relatively long atmospheric lifetime and a high global warming potential. The U.S. is thought to contribute substantially to global SO 2 F 2 emissions, but there is a paucity of information on how emissions of SO 2 F 2 are distributed across the U.S., and there is currently no inventory of SO 2 F 2 emissions for the U.S. or individual states. Here we provide an atmospheric measurement-based estimate of U.S. SO 2 F 2 emissions using high-precision SO 2 F 2 measurements from the NOAA Global Greenhouse Gas Reference Network (GGGRN) and a geostatistical inverse model. We find that California has the largest SO 2 F 2 emissions among all U.S. states, with the highest emissions from southern coastal California (Los Angeles, Orange, and San Diego counties). Outside of California, only very small and infrequent SO 2 F 2 emissions are detected by our analysis of GGGRN data. We find that California emits 60-85% of U.S. SO 2 F 2 emissions, at a rate of 0.26 ( ± 0.10) Gg yr −1 . We estimate that emissions of SO 2 F 2 from California are equal to 5.5–12% of global SO 2 F 2 emissions.

Despite the key role of the Arctic in the global Earth system, year-round in-situ atmospheric composition observations within the Arctic are sparse and mostly rely on measurements at ground-based coastal stations. Measurements of a suite of in-situ trace gases were performed in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. These observations give a comprehensive picture of year-round near-surface atmospheric abundances of key greenhouse and trace gases, i.e., carbon dioxide, methane, nitrous oxide, ozone, carbon monoxide, dimethylsulfide, sulfur dioxide, elemental mercury, and selected volatile organic compounds (VOCs). Redundancy in certain measurements supported continuity and permitted cross-evaluation and validation of the data. This paper gives an overview of the trace gas measurements conducted during MOSAiC and highlights the high quality of the monitoring activities. In addition, in the case of redundant measurements, merged datasets are provided and recommended for further use by the scientific community. Measurement(s) atmospheric ozone • atmospheric carbon dioxide • atmospheric methane • atmospheric carbon monoxide • atmospheric nitrous oxide • atmospheric dimethylsulfide • atmospheric sulfur dioxide • atmospheric gaseous elemental mercury • volatile organic compounds Technology Type(s) ozone analyzer • carbon dioxide analyzer • methane analyzer • carbon monoxide analyzer • nitrous oxide analyzer • dimethylsulfide analyzer • sulfur dioxide analyzer • gaseous elemental mercury analyzer • gas chromatography-mass spectrometry Sample Characteristic - Environment Atmosphere Sample Characteristic - Location central Arctic

We present measurements of CO mole fraction and CO stable isotopes (δ13CO and δC18O) in air during the winters of 2013–14 and 2014–15 at tall tower sampling sites in and around Indianapolis, USA. A tower located upwind of the city was used to quantitatively remove the background CO signal, allowing for the first unambiguous isotopic characterization of the urban CO source and yielding 13CO of –27.7 ± 0.5‰ VPDB and C18O of 17.7 ± 1.1‰ VSMOW for this source. We use the tower isotope measurements, results from a limited traffic study, as well as atmospheric reaction rates to examine contributions from different sources to the Indianapolis CO budget. Our results are consistent with earlier findings that traffic emissions are the dominant source, suggesting a contribution of 96% or more to the overall Indianapolis wintertime CO emissions. Our results are also consistent with the hypothesis that emissions from a small fraction of vehicles without functional catalytic systems dominate the Indianapolis CO budget.

The production of chlorofluorocarbons (CFCs) that would ultimately be released to the atmosphere was banned globally in 2010 under the Montreal Protocol. Here we use measurements combined with an atmospheric transport model to show how atmospheric abundances and emissions of five CFCs increased between 2010 and 2020, contrary to the goals of the phase-out. The Montreal Protocol allows CFC production for use as a feedstock to produce other chemicals. Emissions of CFC-113a, CFC-114a and CFC-115 probably arise during the production of hydrofluorocarbons, which have replaced CFCs for many applications. The drivers behind increasing emissions of CFC-13 and CFC-112a are more uncertain. The combined emissions of CFC-13, CFC-112a, CFC-113a, CFC-114a and CFC-115 increased from 1.6 ± 0.2 to 4.2 ± 0.4 ODP-Gg yr-1 (CFC-11-equivalent ozone-depleting potential) between 2010 and 2020. The anticipated impact of these emissions on stratospheric ozone recovery is small. However, ongoing emissions of the five CFCs of focus may negate some of the benefits gained under the Montreal Protocol if they continue to rise. In addition, the climate impact of the emissions of these CFCs needs to be considered, as their 2020 emissions are equivalent to 47 ± 5 TgCO2.Levels of five chlorofluorocarbons rose in the atmosphere from 2010 to 2020 despite their production being banned by the Montreal Protocol, probably arising as by-products of hydrofluorocarbon production, according to analysis of abundance and emissions data.

The hydroxyl radical (OH) largely determines the atmosphere's oxidative capacity and, thus, the lifetimes of numerous trace gases, including methane (CH4). Hitherto, observation-based approaches for estimating the atmospheric oxidative capacity have primarily relied on using methyl chloroform (MCF), but as the atmospheric abundance of MCF has declined, the uncertainties associated with this method have increased. In this study, we examine the use of five hydrofluorocarbons (HFCs) (HFC-134a, HFC-152a, HFC-365mfc, HFC-245fa, and HFC-32) in multi-species inversions, which assimilate three HFCs simultaneously, as an alternative method to estimate atmospheric OH. We find robust estimates of OH regardless of which combination of the three HFCs are used in the inversions. Our results show that OH has remained fairly stable during our study period from 2004 to 2021, with variations of

In the Arctic and Boreal region (ABR) where warming is especially pronounced, the increase of gross primary production (GPP) has been suggested as an important driver for the increase of the atmospheric CO₂ seasonal cycle amplitude (SCA). However, the role of GPP relative to changes in ecosystem respiration (ER) remains unclear, largely due to our inability to quantify these gross fluxes on regional scales. Here, we use atmospheric carbonyl sulfide (COS) measurements to provide observation-based estimates of GPP over the North American ABR. Our annual GPP estimate is 3.6 (2.4 to 5.5) PgC · y−1 between 2009 and 2013, the uncertainty of which is smaller than the range of GPP estimated from terrestrial ecosystem models (1.5 to 9.8 PgC · y−1). Our COS-derived monthly GPP shows significant correlations in space and time with satellite-based GPP proxies, solar-induced chlorophyll fluorescence, and near-infrared reflectance of vegetation. Furthermore, the derived monthly GPP displays two different linear relationships with soil temperature in spring versus autumn, whereas the relationship between monthly ER and soil temperature is best described by a single quadratic relationship throughout the year. In spring to midsummer, when GPP is most strongly correlated with soil temperature, our results suggest the warming-induced increases of GPP likely exceeded the increases of ER over the past four decades. In autumn, however, increases of ER were likely greater than GPP due to light limitations on GPP, thereby enhancing autumn net carbon emissions. Both effects have likely contributed to the atmospheric CO₂ SCA amplification observed in the ABR.

Global emissions of the ozone-depleting gas HCFC-141b (1,1-dichloro-1-fluoroethane, CH3CCl2F) derived from measurements of atmospheric mole fractions increased between 2017 and 2021 despite a fall in reported production and consumption of HCFC-141b for dispersive uses. HCFC-141b is a controlled substance under the Montreal Protocol, and its phase-out is currently underway, after a peak in reported consumption and production in developing (Article 5) countries in 2013. If reported production and consumption are correct, our study suggests that the 2017–2021 rise is due to an increase in emissions from the bank when appliances containing HCFC-141b reach the end of their life, or from production of HCFC-141b not reported for dispersive uses. Regional emissions have been estimated between 2017–2020 for all regions where measurements have sufficient sensitivity to emissions. This includes the regions of northwestern Europe, east Asia, the United States and Australia, where emissions decreased by a total of 2.3 ± 4.6 Gg yr−1, compared to a mean global increase of 3.0 ± 1.2 Gg yr−1 over the same period. Collectively these regions only account for around 30 % of global emissions in 2020. We are not able to pinpoint the source regions or specific activities responsible for the recent global emission rise.

The Montreal Protocol and its successive amendments have been successful in curbing emissions of ozone-depleting substances and potent greenhouse gases via production/consumption controls. Here we show that the radiative forcing and equivalent effective chlorine from hydrochlorofluorocarbons has decreased from 61.75 mW m − 2 and 321.69 ppt, respectively, since 2021, 5 years before the most recent projected decrease. This important milestone demonstrates the benefits of the Protocol for mitigating climate change and stratospheric ozone layer loss. Hydrochlorofluorocarbons are important ozone-depleting substances. Here the authors show that the radiative forcing and equivalent effective chlorine from hydrochlorofluorocarbons has decreased in recent years, 5 years earlier than expected.