89 research outputs found
Modelling the growth of atmospheric nitrous oxide using a global hierarchical inversion
Nitrous oxide is a potent greenhouse gas (GHG) and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions, which includes prior emissions with truncated Gaussian distributions and Gaussian model errors, in order to examine the drivers of the atmospheric surface growth rate. We show that both emissions and climatic variability are key drivers of variations in the surface nitrous oxide growth rate between 2011 and 2020. We derive increasing global nitrous oxide emissions, which are mainly driven by emissions between 0 and 30∘ N, with the highest emissions recorded in 2020. Our mean global total emissions for 2011–2020 of 17.2 (16.7–17.7 at the 95 % credible intervals) Tg N yr−1, comprising of 12.0 (11.2–12.8) Tg N yr−1 from land and 5.2 (4.5–5.9) Tg N yr−1 from ocean, agrees well with previous studies, but we find that emissions are poorly constrained for some regions of the world, particularly for the oceans. The prior emissions used in this and other previous work exhibit a seasonal cycle in the extra-tropical Northern Hemisphere that is out of phase with the posterior solution, and there is a substantial zonal redistribution of emissions from the prior to the posterior. Correctly characterizing the uncertainties in the system, for example in the prior emission fields, is crucial for deriving posterior fluxes that are consistent with observations. In this hierarchical inversion, the model-measurement discrepancy and the prior flux uncertainty are informed by the data, rather than solely through “expert judgement”. We show cases where this framework provides different plausible adjustments to the prior fluxes compared to inversions using widely adopted, fixed uncertainty constraints.</p
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Modelling the growth of atmospheric nitrous oxide using a global hierarchical inversion
Nitrous oxide is a potent greenhouse gas (GHG) and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions, which includes prior emissions with truncated Gaussian distributions and Gaussian model errors, in order to examine the drivers of the atmospheric surface growth rate. We show that both emissions and climatic variability are key drivers of variations in the surface nitrous oxide growth rate between 2011 and 2020. We derive increasing global nitrous oxide emissions, which are mainly driven by emissions between 0 and 30∘ N, with the highest emissions recorded in 2020. Our mean global total emissions for 2011–2020 of 17.2 (16.7–17.7 at the 95 % credible intervals) Tg N yr−1, comprising of 12.0 (11.2–12.8) Tg N yr−1 from land and 5.2 (4.5–5.9) Tg N yr−1 from ocean, agrees well with previous studies, but we find that emissions are poorly constrained for some regions of the world, particularly for the oceans. The prior emissions used in this and other previous work exhibit a seasonal cycle in the extra-tropical Northern Hemisphere that is out of phase with the posterior solution, and there is a substantial zonal redistribution of emissions from the prior to the posterior. Correctly characterizing the uncertainties in the system, for example in the prior emission fields, is crucial for deriving posterior fluxes that are consistent with observations. In this hierarchical inversion, the model-measurement discrepancy and the prior flux uncertainty are informed by the data, rather than solely through “expert judgement”. We show cases where this framework provides different plausible adjustments to the prior fluxes compared to inversions using widely adopted, fixed uncertainty constraints.</p
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Global emissions of perfluorocyclobutane (PFC-318, c-C4F8) resulting from the use of hydrochlorofluorocarbon-22 (HCFC-22) feedstock to produce polytetrafluoroethylene (PTFE) and related fluorochemicals
Abstract. Emissions of the potent greenhouse gas perfluorocyclobutane
(c-C4F8, PFC-318, octafluorocyclobutane) into the global atmosphere
inferred from atmospheric measurements have been increasing sharply since
the early 2000s. We find that these inferred emissions are highly correlated
with the production of hydrochlorofluorocarbon-22 (HCFC-22, CHClF2) for
feedstock (FS) uses, because almost all HCFC-22 FS is pyrolyzed to produce
(poly)tetrafluoroethylene ((P)TFE) and hexafluoropropylene (HFP), a process
in which c-C4F8 is a known by-product, causing a significant
fraction of global c-C4F8 emissions. We find a global emission
factor of ∼0.003 kg c-C4F8 per kilogram of HCFC-22 FS
pyrolyzed. Mitigation of these c-C4F8 emissions, e.g., through
process optimization, abatement, or different manufacturing processes, such
as refined methods of electrochemical fluorination and waste recycling,
could reduce the climate impact of this industry. While it has been shown
that c-C4F8 emissions from developing countries dominate global
emissions, more atmospheric measurements and/or detailed process statistics
are needed to quantify c-C4F8 emissions at country to facility
levels
Global trends and European emissions of tetrafluoromethane (CF4), hexafluoroethane (C2F6) and octafluoropropane (C3F8)
Perfluorocarbons (PFCs) are amongst the most potent greenhouse gases listed under the United Nations Framework Convention on Climate Change (UNFCCC). With atmospheric lifetimes on the order of thousands to tens of thousands of years, PFC emissions represent a permanent alteration to the global atmosphere on human timescales. While the industries responsible for the vast majority of these emissions-aluminium smelting and semi-conductor manufacturing-have made efficiency improvements and introduced abatement measures, the global mean mole fractions of three PFCs, namely tetrafluoromethane (CF4, PFC-14), hexafluoroethane (C2F6, PFC-116) and octafluoropropane (C3F8, PFC-218), continue to grow. In this study, we update baseline growth rates using in situ high-frequency measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and, using data from four European stations, estimate PFC emissions for northwest Europe. The global growth rate of CF4 decreased from 1.3 ppt yr-1 in 1979 to 0.6 ppt yr-1 around 2010 followed by a renewed steady increase to 0.9 ppt yr-1 in 2019. For C2F6, the growth rate grew to a maximum of 0.125 ppt yr-1 around 1999, followed by a decline to a minimum of 0.075 ppt yr-1 in 2009, followed by weak growth thereafter. The C3F8 growth rate was around 0.007 ppt yr-1 until the early 1990s and then quickly grew to a maximum of 0.03 ppt yr-1 in 2003-2004. Following a period of decline until 2012 to 0.015 ppt yr-1, the growth rate slowly increased again to ∼ 0.017 ppt yr-1 in 2019. We used an inverse modelling framework to infer PFC emissions for northwest Europe. No statistically significant trend in regional emissions was observed for any of the PFCs assessed. For CF4, European emissions in early years were linked predominantly to the aluminium industry. However, we link large emissions in recent years to a chemical manufacturer in northwest Italy. Emissions of C2F6 are linked to a range of sources, including a semi-conductor manufacturer in Ireland and a cluster of smelters in Germany's Ruhr valley. In contrast, northwest European emissions of C3F8 are dominated by a single source in northwest England, raising the possibility of using emissions from this site for a tracer release experiment
Quantifying aluminum and semiconductor industry perfluorocarbon emissions from atmospheric measurements
Atmospheric abundance and global emissions of perfluorocarbons CF4, C2F6 and C3F8 since 1800 inferred from ice core, firn, air archive and in situ measurements
Perfluorocarbons (PFCs) are very potent and long-lived greenhouse gases in the atmosphere, released predominantly during aluminium production and semiconductor manufacture. They have been targeted for emission controls under the United Nations Framework Convention on Climate Change. Here we present the first continuous records of the atmospheric abundance of CF4 (PFC-14), C2F6 (PFC-116) and C3F8 (PFC-218) from 1800 to 2014. The records are derived from high-precision measurements of PFCs in air extracted from polar firn or ice at six sites (DE08, DE08-2, DSSW20K, EDML, NEEM and South Pole) and air archive tanks and atmospheric air sampled from both hemispheres. We take account of the age characteristics of the firn and ice core air samples and demonstrate excellent consistency between the ice core, firn and atmospheric measurements. We present an inversion for global emissions from 1900 to 2014. We also formulate the inversion to directly infer emission factors for PFC emissions due to aluminium production prior to the 1980s. We show that 19th century atmospheric levels, before significant anthropogenic influence, were stable at 34.1 ± 0.3 ppt for CF4 and below detection limits of 0.002 and 0.01 ppt for C2F6 and C3F8, respectively. We find a significant peak in CF4 and C2F6 emissions around 1940, most likely due to the high demand for aluminium during World War II, for example for construction of aircraft, but these emissions were nevertheless much lower than in recent years. The PFC emission factors for aluminium production in the early 20th century were significantly higher than today but have decreased since then due to improvements and better control of the smelting process. Mitigation efforts have led to decreases in emissions from peaks in 1980 (CF4) or early-to-mid-2000s (C2F6 and C3F8) despite the continued increase in global aluminium production; however, these decreases in emissions appear to have recently halted. We see a temporary reduction of around 15 % in CF4 emissions in 2009, presumably associated with the impact of the global financial crisis on aluminium and semiconductor production
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Instruments and Methods: A novel method for obtaining very large ancient air samples from ablating glacial ice for analyses of methane radiocarbon
We present techniques for obtaining large (∼100 L STP) samples of ancient air for analysis of ¹⁴C of methane (¹⁴CH₄) and other trace constituents. Paleoatmospheric ¹⁴CH₄ measurements should constrain the fossil fraction of past methane budgets, as well as provide a definitive test of methane clathrate involvement in large and rapid methane concentration ([CH₄]) increases that accompanied rapid warming events during the last deglaciation. Air dating to the Younger Dryas-Preboreal and Oldest Dryas-Bølling abrupt climatic transitions was obtained by melt extraction from old glacial ice outcropping at an ablation margin in West Greenland. The outcropping ice and occluded air were dated using a combination of δ¹⁵N of N₂, δ¹⁸O of O₂, δ¹⁸O[subscript ice] and [CH₄] measurements. The [CH₄] blank of the melt extractions was <4 ppb. Measurements of δ¹⁸O and δ¹⁵N indicated no significant gas isotopic fractionation from handling. Measured Ar/N₂, CFC-11 and CFC-12 in the samples indicated no significant contamination from ambient air. Ar/N₂, Kr/Ar and Xe/Ar ratios in the samples were used to quantify effects of gas dissolution during the melt extractions and correct the sample [CH₄]. Corrected [CH₄] is elevated over expected values by up to 132 ppb for most samples, suggesting some in situ CH₄ production in ice at this site.This is the publisher’s final pdf. The published article is copyrighted by the International Glaciological Society and can be found at: http://www.igsoc.org/journal
Evidence of a recent decline in UK emissions of hydrofluorocarbons determined by the InTEM inverse model and atmospheric measurements
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 35ĝ€¯%, indicating progress toward the target of a 79ĝ€¯% decrease in sales by 2030. The total InTEM HFC emission estimates (2008-2018) are on average 73 (62-83)ĝ€¯% of, or 4.3 (2.7-5.9)ĝ€¯Tgĝ€¯CO2-eqĝ€¯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.</p
Using ice core measurements from Taylor Glacier, Antarctica, to calibrate in situ cosmogenic 14 C production rates by muons
Cosmic rays entering the Earth’s atmosphere produce showers of secondary particles such as protons, neutrons, and muons. The interaction of these particles with oxygen-16 (16O) in minerals such as ice and quartz can produce carbon-14 (14C). In glacial ice, 14C is also incorporated through trapping of 14C-containing atmospheric gases (14CO2, 14CO, and 14CH4). Understanding the production rates of in situ cosmogenic 14C is important to deconvolve the in situ cosmogenic and atmospheric 14C signals in ice, both of which contain valuable paleoenvironmental information. Unfortunately, the in situ 14C production rates by muons (which are the dominant production mechanism at depths of > 6m solid ice equivalent) are uncertain. In this study, we use measurements of in situ 14C in ancient ice (> 50 ka) from the Taylor Glacier, an ablation site in Antarctica, in combination with a 2D ice flow model to better constrain the compound-specific rates of 14C production by muons and the partitioning of in situ 14C between CO2, CO, and CH4. Our measurements show that 33.7% (11.4%; 95% confidence interval) of the produced cosmogenic 14C forms 14CO and 66.1% (11.5%; 95% confidence interval) of the produced cosmogenic 14C forms 14CO2. 14CH4 represents a very small fraction (< 0.3%) of the total. Assuming that the majority of in situ muogenic 14C in ice forms 14CO2, 14CO, and 14CH4, we also calculated muogenic 14C production rates that are lower by factors of 5.7 (3.6–13.9; 95% confidence interval) and 3.7 (2.0–11.9; 95% confidence interval) for negative muon capture and fast muon interactions, respectively, when compared to values determined in quartz from laboratory studies (Heisinger et al., 2002a, b) and in a natural setting (Lupker et al., 2015). This apparent discrepancy in
muogenic 14C production rates in ice and quartz currently lacks a good explanation and requires further investigation
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