scholarly journals Australian chlorofluorocarbon (CFC) emissions: 1960–2017

2020 ◽  
Vol 17 (8) ◽  
pp. 525
Author(s):  
Paul J. Fraser ◽  
Bronwyn L. Dunse ◽  
Paul B. Krummel ◽  
L. Paul Steele ◽  
Nada Derek ◽  
...  
Keyword(s):  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Small Contribution ◽  
Temporal Behaviour ◽  
Closed Cell ◽  
Production And Consumption ◽  
Consumption Data ◽  
Conditioning Equipment ◽  
Australian Greenhouse ◽  
Atmospheric Concentrations

Environmental contextChlorofluorocarbons (CFCs) are potent greenhouse and stratospheric ozone depleting trace gases. Their atmospheric concentrations are in decline, thanks to global production and consumption controls imposed by the Montreal Protocol. In recent years, the rates of decline of CFC atmospheric concentrations, especially for CFC-11 (CCl3F), are not as large as anticipated under the Protocol, resulting in renewed efforts to estimate CFC consumption and/or emissions to possibly identify new or poorly quantified sources. AbstractAustralian emissions of chlorofluorocarbons (CFCs) have been estimated from atmospheric CFC observations by both inverse modelling and interspecies correlation techniques, and from CFC production, import and consumption data compiled by industry and government. Australian and global CFC emissions show similar temporal behaviour, with emissions peaking in the late-1980s and then declining by ~10% per year through to the present. Australian CFC emissions since 1978 account for less than 1% of global emissions and therefore make a correspondingly small contribution to stratospheric ozone depletion. The current CFC emissions in Australia are likely from ‘banks’ of closed-cell foams, and refrigeration–air conditioning equipment now more than 20 years old. There is no evidence of renewed consumption or emissions of CFCs in Australia. The reduction in CFC emissions has made a significant contribution to reducing Australian greenhouse gas emissions.

scholarly journals CCl<sub>4</sub> distribution derived from MIPAS ESA v7 data: intercomparisons, trend, and lifetime estimation

2017 ◽  
Vol 17 (16) ◽  
pp. 10143-10162 ◽  
Author(s):  
Massimo Valeri ◽  
Flavio Barbara ◽  
Chris Boone ◽  
Simone Ceccherini ◽  
Marco Gai ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Michelson Interferometer ◽  
Montreal Protocol ◽  
Average Lifetime ◽  
Atmospheric Emissions ◽  
Upper Troposphere ◽  
Production And Consumption ◽  
Atmospheric Observations ◽  
Surface Measurements ◽  
Atmospheric Concentrations

Abstract. Atmospheric emissions of carbon tetrachloride (CCl4) are regulated by the Montreal Protocol due to its role as a strong ozone-depleting substance. The molecule has been the subject of recent increased interest as a consequence of the so-called mystery of CCl4, the discrepancy between atmospheric observations and reported production and consumption. Surface measurements of CCl4 atmospheric concentrations have declined at a rate almost 3 times lower than its lifetime-limited rate, suggesting persistent atmospheric emissions despite the ban. In this paper, we study CCl4 vertical and zonal distributions in the upper troposphere and lower stratosphere (including the photolytic loss region, 70–20 hPa), its trend, and its stratospheric lifetime using measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), which operated onboard the ENVISAT satellite from 2002 to 2012. Specifically, we use the MIPAS data product generated with Version 7 of the Level 2 algorithm operated by the European Space Agency.The CCl4 zonal means show features typical of long-lived species of anthropogenic origin that are destroyed primarily in the stratosphere, with larger quantities in the troposphere and a monotonic decrease with increasing altitude in the stratosphere. MIPAS CCl4 measurements have been compared with independent measurements from other satellite and balloon-borne remote sounders, showing a good agreement between the different datasets.CCl4 trends are calculated as a function of both latitude and altitude. Negative trends of about −10 to −15 pptv decade−1 (−10 to −30 % decade−1) are found at all latitudes in the upper troposphere–lower stratosphere region, apart from a region in the southern midlatitudes between 50 and 10 hPa where the trend is positive with values around 5–10 pptv decade−1 (15–20 % decade−1). At the lowest altitudes sounded by MIPAS, we find trends consistent with those determined on the basis of long-term ground-based measurements (−10 to −13 pptv decade−1). For higher altitudes, the trend shows a pronounced asymmetry between the Northern and Southern hemispheres, and the magnitude of the decline rate increases with altitude. We use a simplified model assuming tracer–tracer linear correlations to determine CCl4 lifetime in the lower stratosphere. The calculation provides a global average lifetime of 47 (39–61) years, considering CFC-11 as the reference tracer. This value is consistent with the most recent literature result of 44 (36–58) years.

scholarly journals Australian carbon tetrachloride emissions in a global context

2014 ◽  
Vol 11 (1) ◽  
pp. 77 ◽  
Author(s):  
Paul J. Fraser ◽  
Bronwyn L. Dunse ◽  
Alistair J. Manning ◽  
Sean Walsh ◽  
R. Hsiang J. Wang ◽  
...  
Keyword(s):  
Carbon Tetrachloride ◽  
Environmental Concern ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Global Network ◽  
Atmospheric Gases ◽  
Global Context ◽  
Production And Consumption ◽  
Atmospheric Observations ◽  
Using Data

Environmental context Carbon tetrachloride in the background atmosphere is a significant environmental concern, responsible for ~10% of observed stratospheric ozone depletion. Atmospheric concentrations of CCl4 are higher than expected from currently identified emission sources: largely residual emissions from production, transport and use. Additional sources are required to balance the expected atmospheric destruction of CCl4 and may contribute to a slower-than-expected recovery of the Antarctic ozone ‘hole’. Abstract Global (1978–2012) and Australian (1996–2011) carbon tetrachloride emissions are estimated from atmospheric observations of CCl4 using data from the Advanced Global Atmospheric Gases Experiment (AGAGE) global network, in particular from Cape Grim, Tasmania. Global and Australian emissions are in decline in response to Montreal Protocol restrictions on CCl4 production and consumption for dispersive uses in the developed and developing world. However, atmospheric data-derived emissions are significantly larger than ‘bottom-up’ estimates from direct and indirect CCl4 production, CCl4 transportation and use. Australian CCl4 emissions are not a result of these sources, and the identification of the origin of Australian emissions may provide a clue to the origin of some of these ‘missing’ global sources.

scholarly journals Biological nitrous oxide consumption in oxygenated waters of the high latitude Atlantic Ocean

2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Andrew P. Rees ◽  
Ian J. Brown ◽  
Amal Jayakumar ◽  
Gennadi Lessin ◽  
Paul J. Somerfield ◽  
...  
Keyword(s):  
Nitrous Oxide ◽  
Atlantic Ocean ◽  
High Latitude ◽  
Bacterial Communities ◽  
Stratospheric Ozone ◽  
Intermediate Step ◽  
Anoxic Environments ◽  
Production And Consumption ◽  
Net Flux ◽  
Traditional Understanding

AbstractNitrous oxide (N2O) is important to the global radiative budget of the atmosphere and contributes to the depletion of stratospheric ozone. Globally the ocean represents a large net flux of N2O to the atmosphere but the direction of this flux varies regionally. Our understanding of N2O production and consumption processes in the ocean remains incomplete. Traditional understanding tells us that anaerobic denitrification, the reduction of NO3− to N2 with N2O as an intermediate step, is the sole biological means of reducing N2O, a process known to occur in anoxic environments only. Here we present experimental evidence of N2O removal under fully oxygenated conditions, coupled with observations of bacterial communities with novel, atypical gene sequences for N2O reduction. The focus of this work was on the high latitude Atlantic Ocean where we show bacterial consumption sufficient to account for oceanic N2O depletion and the occurrence of regional sinks for atmospheric N2O.

scholarly journals Changing trends and emissions of hydrochlorofluorocarbons and their hydrofluorocarbon replacements

2016 ◽  
Author(s):  
Peter G. Simmonds ◽  
Matthew Rigby ◽  
Archibold McCulloch ◽  
Simon O'Doherty ◽  
Dickon Young ◽  
...  
Keyword(s):  
Growth Rates ◽  
Montreal Protocol ◽  
Hfc 134A ◽  
Production And Consumption ◽  
Ozone Depleting Substances ◽  
Phase Out ◽  
Article 5 ◽  
The Impact ◽  
Global Emissions

Abstract. 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. The 2007 adjustment to the Montreal Protocol required the accelerated phase-out 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 reduction in global emissions of the four HCFCs with aggregated global emissions in 2015 of 444 ± 75 Gg/yr, in CO2 equivalent units (CO2 e) 0.75 ± 0.1 Gt/yr, compared with 483 ± 70 Gg/yr (0.82 ± 0.1 Gt/yr CO2 e) in 2010. (All quoted uncertainties in this paper are 1 sigma). About 80 % of the total HCFC atmospheric burden in 2015 is HCFC-22, where global HCFC emissions appear to have been relatively constant in spite of the 2013 cap on global production and consumption. 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 annual growth rates with aggregated global HFCs emissions in 2015 of 329 ± 70 Gg/yr (0.65 ± 0.12 Gt/yr CO2 e) compared to 2010 with 240 ± 50 Gg/yr (0.47 ± 0.08 Gt/yr CO2 e). As HCFCs are replaced by HFCs we investigate the impact of the shift to refrigerant blends which have lower global warming potentials (GWPs). We also note that emissions of HFC-125 and HFC-32 appear to have increased more rapidly during the 2011–2015 5-yr period compared to 2006–2010.

scholarly journals Estimates of European emissions of methyl chloroform using a Bayesian inversion method

2014 ◽  
Vol 14 (18) ◽  
pp. 9755-9770 ◽  
Author(s):  
M. Maione ◽  
F. Graziosi ◽  
J. Arduini ◽  
F. Furlani ◽  
U. Giostra ◽  
...  
Keyword(s):  
Point Source ◽  
High Frequency ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Source Analysis ◽  
Bayesian Inversion ◽  
Inversion Method ◽  
Data Set ◽  
Methyl Chloroform

Abstract. Methyl chloroform (MCF) is a man-made chlorinated solvent contributing to the destruction of stratospheric ozone and is controlled under the "Montreal Protocol on Substances that Deplete the Ozone Layer" and its amendments, which called for its phase-out in 1996 in developed countries and 2015 in developing countries. Long-term, high-frequency observations of MCF carried out at three European sites show a constant decline in the background mixing ratios of MCF. However, we observe persistent non-negligible mixing ratio enhancements of MCF in pollution episodes, suggesting unexpectedly high ongoing emissions in Europe. In order to identify the source regions and to give an estimate of the magnitude of such emissions, we have used a Bayesian inversion method and a point source analysis, based on high-frequency long-term observations at the three European sites. The inversion identified southeastern France (SEF) as a region with enhanced MCF emissions. This estimate was confirmed by the point source analysis. We performed this analysis using an 11-year data set, from January 2002 to December 2012. Overall, emissions estimated for the European study domain decreased nearly exponentially from 1.1 Gg yr−1 in 2002 to 0.32 Gg yr−1 in 2012, of which the estimated emissions from the SEF region accounted for 0.49 Gg yr−1 in 2002 and 0.20 Gg yr−1 in 2012. The European estimates are a significant fraction of the total semi-hemisphere (30–90° N) emissions, contributing a minimum of 9.8% in 2004 and a maximum of 33.7% in 2011, of which on average 50% are from the SEF region. On the global scale, the SEF region is thus responsible for a minimum of 2.6% (in 2003) and a maximum of 10.3% (in 2009) of the global MCF emissions.

scholarly journals Stratospheric ozone interannual variability (1995–2011) as observed by Lidar and Satellite at Mauna Loa Observatory, HI and Table Mountain Facility, CA

2012 ◽  
Vol 12 (11) ◽  
pp. 30825-30867
Author(s):  
G. Kirgis ◽  
T. Leblanc ◽  
I. S. McDermid ◽  
T. D. Walsh
Keyword(s):  
Time Series ◽  
Solar Cycle ◽  
Interannual Variability ◽  
Southern Oscillation ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Quasi Biennial Oscillation ◽  
Mauna Loa ◽  
Table Mountain ◽  
Biennial Oscillation

Abstract. The Jet Propulsion Laboratory (JPL) lidars, at the Mauna Loa Observatory, Hawaii (MLO, 19.5° N, 155.6° W) and the JPL Table Mountain Facility (TMF, California, 34.5° N, 117.7° W), have been measuring vertical profiles of stratospheric ozone routinely since the early 1990's and late-1980s respectively. Interannual variability of ozone above these two sites was investigated using a multi-linear regression analysis on the deseasonalized monthly mean lidar and satellite time-series at 1 km intervals between 20 and 45 km from January 1995 to April 2011, a period of low volcanic aerosol loading. Explanatory variables representing the 11-yr solar cycle, the El Niño Southern Oscillation, the Quasi-Biennial Oscillation, the Eliassen–Palm flux, and horizontal and vertical transport were used. A new proxy, the mid-latitude ozone depleting gas index, which shows a decrease with time as an outcome of the Montreal Protocol, was introduced and compared to the more commonly used linear trend method. The analysis also compares the lidar time-series and a merged time-series obtained from the space-borne stratospheric aerosol and gas experiment II, halogen occultation experiment, and Aura-microwave limb sounder instruments. The results from both lidar and satellite measurements are consistent with recent model simulations which propose changes in tropical upwelling. Additionally, at TMF the ozone depleting gas index explains as much variance as the Quasi-Biennial Oscillation in the upper stratosphere. Over the past 17 yr a diminishing downward trend in ozone was observed before 2000 and a net increase, and sign of ozone recovery, is observed after 2005. Our results which include dynamical proxies suggest possible coupling between horizontal transport and the 11-yr solar cycle response, although a dataset spanning a period longer than one solar cycle is needed to confirm this result.

scholarly journals How sensitive is the recovery of stratospheric ozone to changes in concentrations of very short-lived bromocarbons?

2014 ◽  
Vol 14 (19) ◽  
pp. 10431-10438 ◽  
Author(s):  
X. Yang ◽  
N. L. Abraham ◽  
A. T. Archibald ◽  
P. Braesicke ◽  
J. Keeble ◽  
...  
Keyword(s):  
Climate Model ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Background Concentrations ◽  
Future Situation ◽  
Antarctic Ozone ◽  
The Antarctic ◽  
The Impact ◽  
Ozone Column ◽  
Policy Question

Abstract. Naturally produced very short-lived substances (VSLS) account for almost a quarter of the current stratospheric inorganic bromine, Bry. Following VSLS oxidation, bromine radicals (Br and BrO) can catalytically destroy ozone. The extent to which possible increases in surface emissions or transport of these VSLS bromocarbons to the stratosphere could counteract the effect of halogen reductions under the Montreal Protocol is an important policy question. Here, by using a chemistry–climate model, UM-UKCA, we investigate the impact of a hypothetical doubling (an increase of 5 ppt Bry) of VSLS bromocarbons on ozone and how the resulting ozone changes depend on the background concentrations of chlorine and bromine. Our model experiments indicate that for the 5 ppt increase in Bry from VSLS, the ozone decrease in the lowermost stratosphere of the Southern Hemisphere (SH) may reach up to 10% in the annual mean; the ozone decrease in the Northern Hemisphere (NH) is smaller (4–6%). The largest impact on the ozone column is found in the Antarctic spring. There is a significantly larger ozone decrease following the doubling of the VSLS burden under a high stratospheric chlorine background than under a low chlorine background, indicating the importance of the inter-halogen reactions. For example, the decline in the high-latitude, lower-stratospheric ozone concentration as a function of Bry is higher by about 30–40% when stratospheric Cly is ~ 3 ppb (present day), compared with Cly of ~ 0.8 ppb (a pre-industrial or projected future situation). Bromine will play an important role in the future ozone layer. However, even if bromine levels from natural VSLS were to increase significantly later this century, changes in the concentration of ozone will likely be dominated by the decrease in anthropogenic chlorine. Our calculation suggests that for a 5 ppt increase in Bry from VSLS, the Antarctic ozone hole recovery date could be delayed by approximately 6–8 years, depending on Cly levels.

Detection of Fourth Generation Synthetic Halocarbons in the Upper Troposphere

2021 ◽  
Author(s):  
Tanja Schuck ◽  
Katharina Meixner ◽  
Peter van Velthoven ◽  
Simon O’Doherty ◽  
Martin Vollmer ◽  
...  
Keyword(s):  
Degradation Products ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Gas Chromatography Mass Spectrometry ◽  
Fourth Generation ◽  
Oh Radicals ◽  
Sample Collection ◽  
Upper Troposphere ◽  
Wide Range ◽  
Air Sample

&lt;p&gt;Synthetic halocarbons are used for a wide range of applications, for example air conditioning or foam blowing. Many of them are long-lived greenhouse gases contributing to climate change and, in addition, may contribute to stratospheric ozone depletion if containing chlorine or bromine. Therefore, their production and use are regulated by the Montreal Protocol and its amendments. These long-lived halocarbons are increasingly replaced by a fourth generation of unsaturated short-lived halocarbons, the hydrochlorofluoroolefines (HCFOs) and hydrofluoroolefines (HFOs). The main removal process of these compounds in the atmosphere is reaction with OH radicals, and their average lifetimes are of the order of up to a few tens of days.&lt;/p&gt;&lt;p&gt;As part of the IAGOS-CARIBIC instrument package we operate an automated air sample collection system during regular flights in the upper troposphere and lowermost stratosphere. At altitudes around 10-12 km, samples are collected in stainless steel and glass flasks at predefined times. Post-flight laboratory analyses include gas chromatography - mass spectrometry measurements of a wide range of halocarbons. The short-lived compounds HFO-1234ze(E) and HCFO-1233zd(E) were detected in a small number of samples, indicating that these compounds are sufficiently long lived for transport into the upper troposphere. There were not found in stratospheric samples.&lt;/p&gt;&lt;p&gt;At this altitude, low abundance of OH and low temperatures may slow down chemical decay, and tracer lifetimes may increase significantly. Based on average temperatures and OH abundance, we estimate local lifetimes of HFO-1234ze(E) and HCFO-1233zd(E)&amp;#160; in the mid-latitudes of up to 75 days and 200 days, respectively. Short-lived H(C)FOs reaching the upper troposphere could thus be transported over large distances and their degradation products may be deposited&amp;#160; far from their emission sources.&lt;/p&gt;

Atmospheric impacts of short-lived chlorinated species over the recent past: a chemistry-climate perspective

2021 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Peter Braesicke ◽  
Martyn Chipperfield
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Lower Boundary ◽  
Montreal Protocol ◽  
Recent Past ◽  
Substantial Impact ◽  
Ozone Depleting Substances ◽  
The Impact

&lt;p&gt;The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl&lt;sub&gt;3&lt;/sub&gt;) and dichloromethane (CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We address this issue using the UM-UKCA chemistry-climate model (CCM). While not only the first, to our knowledge, model study addressing this problem using a CCM, it is also the first such study employing a whole atmosphere model, thereby simulating the tropospheric Cl-VSLSs emissions and the resulting stratospheric impacts in a fully consistent manner. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;We examine the impacts of rising Cl-VSLSs emissions on atmospheric chlorine tracers and ozone, including their long-term trends. We pay particular attention to the role of &amp;#8216;nudging&amp;#8217;, as opposed to the free-running model set up, for the simulated Cl-VSLSs impacts, thereby demostrating the role of atmospheric dynamics in modulating the atmospheric responses to Cl-VSLSs. In addition, we employ novel estimates of Cl-VSLS emissions over the recent past and compare the results with the simulations that prescribe Cl-VSLSs using simple lower boundary conditions. This allows us to demonstrate the impact such choice has on the dominant location and seasonality of the Cl-VSLSs transport into the stratosphere.&lt;/p&gt;

scholarly journals Emissions of Carbon Tetrachloride (CCl<sub>4</sub>) from Europe

2016 ◽  
Author(s):  
Francesco Graziosi ◽  
Jgor Arduini ◽  
Paolo Bonasoni ◽  
Francesco Furlani ◽  
Umberto Giostra ◽  
...  
Keyword(s):  
Carbon Tetrachloride ◽  
Large Scale ◽  
Stratospheric Ozone ◽  
Montreal Protocol ◽  
Scale Production ◽  
Top Down ◽  
Significant Discrepancy ◽  
Bottom Up ◽  
Atmospheric Observations ◽  
Global Emissions

Abstract. Carbon tetrachloride (CCl4) is a long-lived radiatively-active compound able to destroy stratospheric ozone. Due to its inclusion in the Montreal Protocol on Substances that Deplete the Ozone Layer, the last two decades have seen a sharp decrease in its large scale emissive use with a consequent decline of its atmospheric mole fractions. However, the Montreal Protocol restrictions do not apply to the use of carbon tetrachloride as feedstock for the production of other chemicals, implying the risk of fugitive emissions from the industry sector. The occurrence of such unintended emissions is suggested by a significant discrepancy between global emissions as derived by reported production and feedstock usage (bottom-up emissions), and those based on atmospheric observations (top-down emissions). In order to better constrain the atmospheric budget of carbon tetrachloride, several studies based on a combination of atmospheric observations and inverse modelling have been conducted in recent years in various regions of the world. This study is focused on the European scale and based on long-term high-frequency observations at three European sites, combined with a Bayesian inversion methodology. We estimated that average European emissions for 2006–2014 were 2.3 (± 0.8) Gg yr−1, with an average decreasing trend of 7.3 % per year. Our analysis identified France as the main source of emissions over the whole study period, with an average contribution to total European emissions of 25 %. The inversion was also able to allow the localisation of emission "hot-spots" in the domain, with major source areas in Southern France, Central England (UK) and Benelux (Belgium, The Netherlands, Luxembourg), where most of industrial scale production of basic organic chemicals are located. According to our results, European emissions correspond to 4.0 % of global emissions for 2006–2012. Together with other regional studies, our results allow a better constraint of the global budget of carbon tetrachloride and a better quantification of the gap between top-down and bottom-up estimates.

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