13 research outputs found
Trends and emissions of six perfluorocarbons in the Northern Hemisphere and Southern Hemisphere
Perfluorocarbons (PFCs) are potent greenhouse gases with global warming potentials up to several thousand times greater than CO2 on a 100-year time horizon. The lack of any significant sinks for PFCs means that they have long atmospheric lifetimes of the order of thousands of years. Anthropogenic production is thought to be the only source for most PFCs. Here we report an update on the global atmospheric abundances of the following PFCs, most of which have for the first time been analytically separated according to their isomers: c-octafluorobutane (c-C4F8), n-decafluorobutane (n-C4F10), n-dodecafluoropentane (n-C5F12), n-tetradecafluorohexane (n-C6F14), and n-hexadecafluoroheptane (n-C7F16). Additionally, we report the first data set on the atmospheric mixing ratios of perfluoro-2-methylpentane (i-C6F14). The existence and significance of PFC isomers have not been reported before, due to the analytical challenges of separating them. The time series spans a period from 1978 to the present. Several data sets are used to investigate temporal and spatial trends of these PFCs: time series of air samples collected at Cape Grim, Australia, from 1978 to the start of 2018; a time series of air samples collected between July 2015 and April 2017 at Tacolneston, UK; and intensive campaign-based sampling collections from Taiwan. Although the remote “background” Southern Hemispheric Cape Grim time series indicates that recent growth rates of most of these PFCs are lower than in the 1990s, we continue to see significantly increasing mixing ratios that are between 6 % and 27 % higher by the end of 2017 compared to abundances measured in 2010. Air samples from Tacolneston show a positive offset in PFC mixing ratios compared to the Southern Hemisphere baseline. The highest mixing ratios and variability are seen in air samples from Taiwan, which is therefore likely situated much closer to PFC sources, confirming predominantly Northern Hemispheric emissions for most PFCs. Even though these PFCs occur in the atmosphere at levels of parts per trillion molar or less, their total cumulative global emissions translate into 833 million metric tonnes of CO2 equivalent by the end of 2017, 23 % of which has been emitted since 2010. Almost two-thirds of the CO2 equivalent emissions within the last decade are attributable to c-C4F8, which currently also has the highest emission rates that continue to grow. Sources of all PFCs covered in this work remain poorly constrained and reported emissions in global databases do not account for the abundances found in the atmosphere
Investigation of East Asian emissions of CFC-11 using atmospheric observations in Taiwan
Recent findings of an unexpected slowdown in the decline of CFC-11 mixing ratios in the atmosphere have led to the conclusion that global CFC-11 emissions have increased over the past decade and have been attributed in part to eastern China. This study independently assesses these findings by evaluating enhancements of CFC-11 mixing ratios in air samples collected in Taiwan between 2014 and 2018. Using the NAME (Numerical Atmospheric Modeling Environment) particle dispersion model, we find the likely source of the enhanced CFC-11 observed in Taiwan to be East China. Other halogenated trace gases were also measured, and there were positive interspecies correlations between CFC-11 and CHCl3, CCl4, HCFC-141b, HCFC-142b, CH2Cl2, and HCFC-22, indicating co-location of the emissions of these compounds. These correlations in combination with published emission estimates of CH2Cl2 and HCFC-22 from China, and of CHCl3 and CCl4 from eastern China, are used to estimate CFC-11 emissions. Within the uncertainties, these estimates do not differ for eastern China and the whole of China, so we combine them to derive a mean estimate that we term as being from "(eastern) China". For 2014-2018, we estimate an emission of 19 ± 5 Gg year-1 (gigagrams per year) of CFC-11 from (eastern) China, approximately one-quarter of global emissions. Comparing this to previously reported CFC-11 emissions estimated for earlier years, we estimate CFC-11 emissions from (eastern) China to have increased by 7 ± 5 Gg year-1 from the 2008-2011 average to the 2014-2018 average, which is 50 ± 40% of the estimated increase in global CFC-11 emissions and is consistent with the emission increases attributed to this region in an earlier study
Abrupt reversal in emissions and atmospheric abundance of HCFC-133a (CF3CH2Cl)
Hydrochlorofluorocarbon HCFC-133a (CF3CH2Cl) is an anthropogenic compound whose consumption for emissive use is restricted under the Montreal Protocol. A recent study showed rapidly increasing atmospheric abundances and emissions. We report that, following this rise, the at- mospheric abundance and emissions have declined sharply in the past three years. We find a Northern Hemisphere HCFC-133a increase from 0.13 ppt (dry air mole fraction in parts-per-trillion) in 2000 to 0.50 ppt in 2012–mid-2013 followed by an abrupt reversal to 0.44 ppt by early 2015. Global emissions derived from these observations peaked at 3.1 kt in 2011, followed by a rapid decline of 0.5 kt yr−2 to 1.5 kt yr−1 in 2014. Sporadic HCFC-133a pollution events are detected in Europe from our high-resolution HCFC-133a records at three European stations, and in Asia from sam- ples collected in Taiwan. European emissions are estimated to be <0.1 kt yr−1 although emission hotspots were identi- fied in France
Enhanced chlorinated very short-lived substances in South East Asia:Potential source regions and source types
Enhancements of the mixing ratios of short-lived halogenated gases were observed in air samples collected at Bachok Marine Research Station (BMRS), Peninsular Malaysia during Northern Hemisphere winters in 2013/2014 and 2015/2016. This study investigates the potential source regions and source types that influenced the variability in chlorinated very short-lived substances (Cl-VSLS) [dichloromethane, 1,2-dichloroethane, trichloromethane, tetrachloroethene] and methyl halides [methyl chloride and methyl bromide]. The UK Met Office’s Numerical Atmospheric Modelling Environment (NAME) dispersion model, was used for tracking the origin of air masses arriving at BMRS. For the purpose of identifying possible sources of these compounds, carbon monoxide (CO) emission data taken from the Representative Concentration Pathway 8.5 were used along with NAME footprints to calculate modelled CO mixing ratios. A correlation analysis between the mixing ratios of measured compounds and the modelled CO from various emission sectors was perform to assess the extent to which emission sectors might be related to the mixing ratios of halogenated gases. The results show that the events of higher mixing ratios were associated with air masses, especially from East China. During the 2013/2014 campaign, the modelled CO from industrial, solvents and agriculture (waste burning on fields) were significantly correlated with the mixing ratios of Cl-VSLS (R > 0.7) and methyl halides (R > 0.40). During the 2015/2016 campaign, the strength of these correlations reduced for Cl-VSLS (R > 0.5) and with no significant correlations for methyl halides. Instead, mixing ratios of methyl halides were correlated (R=0.4) with modelled CO from forest burning. This work provides evidence that East and South East Asia act as important sources of halogenated gases. This is of significant given the proximity of these regions to prevalent deep convection which can rapidly transport these halogen-containing gases into the stratosphere and impact the ozone layer
Synthetic Triterpenoid Inhibition of Human Ghrelin <i>O</i>‑Acyltransferase: The Involvement of a Functionally Required Cysteine Provides Mechanistic Insight into Ghrelin Acylation
The
peptide hormone ghrelin plays a key role in regulating hunger
and energy balance within the body. Ghrelin signaling presents a promising
and unexploited target for development of small molecule therapeutics
for treatment of obesity, diabetes, and other health conditions. Inhibition
of ghrelin <i>O</i>-acyltransferase (GOAT), which catalyzes
an essential octanoylation step in ghrelin maturation, offers a potential
avenue for controlling ghrelin signaling. Through screening a small
molecule library, we have identified a class of synthetic triterpenoids
that efficiently inhibit ghrelin acylation by the human isoform of
GOAT (hGOAT). These compounds function as covalent reversible inhibitors
of hGOAT, providing the first evidence of the involvement of a nucleophilic
cysteine residue in substrate acylation by a MBOAT family acyltransferase.
Surprisingly, the mouse form of GOAT does not exhibit susceptibility
to cysteine-modifying electrophiles, revealing an important distinction
in the activity and behavior between these closely related GOAT isoforms.
This study establishes these compounds as potent small molecule inhibitors
of ghrelin acylation and provides a foundation for the development
of novel hGOAT inhibitors as therapeutics targeting diabetes and obesity