scholarly journals Re-evaluation of the lifetimes of the major CFCs and CH<sub>3</sub>CCl<sub>3</sub> using atmospheric trends

2012 ◽  
Vol 12 (9) ◽  
pp. 24469-24499 ◽  
Author(s):  
M. Rigby ◽  
R. G. Prinn ◽  
S. O'Doherty ◽  
S. A. Montzka ◽  
A. McCulloch ◽  
...  

Abstract. Since the Montreal Protocol on substances that deplete the ozone layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, therefore the rate at which this recovery occurs will depend largely on the atmospheric lifetime of these compounds. The first ODS measurements began in the early 1970s along with the first lifetime estimates calculated by considering their atmospheric trends. We now have global mole fraction records spanning multiple decades, prompting this lifetime re-evaluation. Using surface measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration Global Monitoring Division (NOAA GMD) from 1978 to 2011, we estimated the lifetime of CFC-11, CFC-12, CFC-113 and CH3CCl3 using a multi-species inverse method. The CFC-11 lifetime of 45 yr, currently recommended in the World Meteorological Organisation (WMO) Scientific Assessment of Ozone Depletion, lies at the lower uncertainty bound of our estimates which are 524066 yr (1-sigma uncertainty) when AGAGE data were used, and 504066 yr when the NOAA network data were used. Our derived lifetime for CFC-113 is higher than the WMO estimates of 85 yr (10488123 using AGAGE, 10387122 using NOAA). Our estimates of the lifetime of CFC-12 and CH3CCl3 agree well with other recent estimates being 10885137 and 10484135 yr (CFC-12, AGAGE and NOAA, respectively) and 5.24.85.6 and 5.24.85.7 yr (CH3CCl3, AGAGE and NOAA, respectively).

2013 ◽  
Vol 13 (5) ◽  
pp. 2691-2702 ◽  
Author(s):  
M. Rigby ◽  
R. G. Prinn ◽  
S. O'Doherty ◽  
S. A. Montzka ◽  
A. McCulloch ◽  
...  

Abstract. Since the Montreal Protocol on Substances that Deplete the Ozone Layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, therefore the rate at which this recovery occurs will depend largely on the atmospheric lifetime of these compounds. The first ODS measurements began in the early 1970s along with the first lifetime estimates calculated by considering their atmospheric trends. We now have global mole fraction records spanning multiple decades, prompting this lifetime re-evaluation. Using surface measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration Global Monitoring Division (NOAA GMD) from 1978 to 2011, we estimated the lifetime of CFC-11, CFC-12, CFC-113 and CH3CCl3 using a multi-species inverse method. A steady-state lifetime of 45 yr for CFC-11, currently recommended in the most recent World Meteorological Organisation (WMO) Scientific Assessments of Ozone Depletion, lies towards the lower uncertainty bound of our estimates, which are 544861 yr (1-sigma uncertainty) when AGAGE data were used and 524561 yr when the NOAA network data were used. Our derived lifetime for CFC-113 is significantly higher than the WMO estimates of 85 yr, being 10999121 (AGAGE) and 10997124 (NOAA). New estimates of the steady-state lifetimes of CFC-12 and CH3CCl3 are consistent with the current WMO recommendations, being 11195132 and 11295136 yr (CFC-12, AGAGE and NOAA respectively) and 5.044.925.20 and 5.044.875.23 yr (CH3CCl3, AGAGE and NOAA respectively).


2021 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Peter Braesicke ◽  
Martyn Chipperfield

&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;


2018 ◽  
Vol 18 (9) ◽  
pp. 6567-6584 ◽  
Author(s):  
Johannes Staehelin ◽  
Pierre Viatte ◽  
Rene Stübi ◽  
Fiona Tummon ◽  
Thomas Peter

Abstract. Climatic Observatory (LKO) in Arosa (Switzerland), marking the beginning of the world's longest series of total (or column) ozone measurements. They were driven by the recognition that atmospheric ozone is important for human health, as well as by scientific curiosity about what was, at the time, an ill characterised atmospheric trace gas. From around the mid-1950s to the beginning of the 1970s studies of high atmosphere circulation patterns that could improve weather forecasting was justification for studying stratospheric ozone. In the mid-1970s, a paradigm shift occurred when it became clear that the damaging effects of anthropogenic ozone-depleting substances (ODSs), such as long-lived chlorofluorocarbons, needed to be documented. This justified continuing the ground-based measurements of stratospheric ozone. Levels of ODSs peaked around the mid-1990s as a result of a global environmental policy to protect the ozone layer, implemented through the 1987 Montreal Protocol and its subsequent amendments and adjustments. Consequently, chemical destruction of stratospheric ozone started to slow around the mid-1990s. To some extent, this raises the question as to whether continued ozone observation is indeed necessary. In the last decade there has been a tendency to reduce the costs associated with making ozone measurements globally including at Arosa. However, the large natural variability in ozone on diurnal, seasonal, and interannual scales complicates the capacity for demonstrating the success of the Montreal Protocol. Chemistry-climate models also predict a super-recovery of the ozone layer at mid-latitudes in the second half of this century, i.e. an increase of ozone concentrations beyond pre-1970 levels, as a consequence of ongoing climate change. These factors, and identifying potentially unexpected stratospheric responses to climate change, support the continued need to document stratospheric ozone changes. This is particularly valuable at the Arosa site, due to the unique length of the observational record. This paper presents the evolution of the ozone layer, the history of international ozone research, and discusses the justification for the measurements in the past, present and into future.


2019 ◽  
pp. 304-322
Author(s):  
Frederike Albrecht ◽  
Charles F. Parker

The Montreal Protocol—the regime designed to protect the stratospheric ozone layer—has widely been hailed as the gold standard of global environmental governance and is one of few examples of international institutional cooperative arrangements successfully solving complex transnational problems. Although the stratospheric ozone layer still bears the impacts of ozone depleting substances (ODSs), the problem of ozone depletion is well on its way to being solved due to the protocol. This chapter examines how the protocol was designed and implemented in a way that has allowed it to successfully overcome a number of thorny challenges that most international environmental regimes must face: how to attract sufficient participation, how to promote compliance and manage non-compliance, how to strengthen commitments over time, how to neutralize or co-opt potential ‘veto players’, how to make the costs of implementation affordable, how to leverage public opinion in support of the regime’s goals, and, ultimately, how to promote the behavioural and policy changes needed to solve the problems and achieve the goals the regime was designed to solve. The chapter concludes that while some of the reasons for the Montreal Protocol’s success, such as fairly affordable, available substitutes for ODSs, are not easy to replicate, there are many other elements of this story that can be utilized when thinking about how to design solutions to other transnational environmental problems.


2020 ◽  
Author(s):  
Brian Zambri ◽  
Susan Solomon ◽  
David Thompson ◽  
Qiang Fu

&lt;p&gt;Ozone depletion in the Southern Hemisphere (SH) stratosphere in the late 20&lt;sup&gt;th&lt;/sup&gt; century cooled the air there, strengthening the SH stratospheric westerly winds near 60&amp;#186;S and altering SH surface climate. Since ~1999, trends in Antarctic ozone have begun to recover, exhibiting a flattening followed by a sign reversal in response to decreases in stratospheric chlorine concentration due to the Montreal Protocol, an international treaty banning the production and consumption of ozone-depleting substances. Here we show that the post&amp;#8211;1999 increase in ozone has resulted in thermal and circulation changes of opposite sign to those that resulted from stratospheric ozone losses, including a warming of the SH polar lower stratosphere and a weakening of the SH stratospheric polar vortex.&amp;#160; Further, these altered trends extend to the upper troposphere, albeit of smaller magnitudes. &amp;#160;Observed post&amp;#8211;1999 trends of temperature and circulation in the stratosphere are about 20&amp;#8211;25% the magnitude of those of the ozone depletion era, and are broadly consistent with expectations based on modeled depletion-era trends and variability of both ozone and reactive chlorine, thereby indicating the emergence of healing of dynamical impacts of the Antarctic ozone hole.&lt;/p&gt;


2019 ◽  
Author(s):  
William T. Ball ◽  
Justin Alsing ◽  
Johannes Staehelin ◽  
Sean M. Davis ◽  
Lucien Froidevaux ◽  
...  

Abstract. The Montreal Protocol has successfully prevented catastrophic losses of stratospheric ozone, and signs of recovery are now evident. Nevertheless, recent work suggests that ozone in the lower stratosphere ( 95 %, 30° S–30° N) decreases dominate the quasi-global integrated decrease (99 % probability); the integrated tropical stratospheric column (1–100 hPa, 30° S–30° N) displays a significant overall decrease, with 95 % probability. These decreases do not reveal an inefficacy of the Montreal Protocol. Rather, they suggest other effects to be at work, mainly dynamical variability on long or short timescale, counteracting the protocol's regulation of halogenated ozone depleting substances (hODS). We demonstrate that large inter-annual mid-latitude variations (30° –60° ), such as the 2017 resurgence, are driven by non-linear QBO phase-dependent seasonal variability. However, this variability is not represented in current regression analyses. To understand if observed lower stratospheric decreases are a transient or long-term phenomenon, progress needs to be made in accounting for this dynamically-driven variability.


2018 ◽  
Vol 18 (2) ◽  
pp. 1379-1394 ◽  
Author(s):  
William T. Ball ◽  
Justin Alsing ◽  
Daniel J. Mortlock ◽  
Johannes Staehelin ◽  
Joanna D. Haigh ◽  
...  

Abstract. Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer–Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60° S and 60° N outside the polar regions (60–90°). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60° S and 60° N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60° S and 60° N. We find that total column ozone between 60° S and 60° N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.


2013 ◽  
Vol 13 (9) ◽  
pp. 4907-4916 ◽  
Author(s):  
A. Voulgarakis ◽  
D. T. Shindell ◽  
G. Faluvegi

Abstract. Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (−22.6 mW m−2 for CFCs and −6.7 mW m−2 for N2O) and sulfate aerosols (−3.0 mW m−2 for CFCs and +6.5 mW m−2 for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.


2013 ◽  
Vol 13 (8) ◽  
pp. 21427-21453
Author(s):  
H. Zhang ◽  
S. Wu ◽  
Y. Wang

Abstract. The stratospheric ozone has decreased greatly since 1980 due to ozone depleting substances (ODSs). As a result of the implementation of the Montreal Protocol and its amendments and adjustments, stratospheric ozone is expected to recover towards its pre-1980 level in the coming decades. We examine the implications of stratospheric ozone recovery for the tropospheric chemistry and ozone air quality with a global chemical transport model (GEOS-Chem). Significant decreases in surface ozone photolysis rates due to stratospheric ozone recovery are simulated. Increases in ozone lifetime by up to 7% are calculated in the troposphere. The global average OH decreases by 1.74% and the global burden of tropospheric ozone increases by 0.78%. The perturbations to tropospheirc ozone and surface ozone show large seasonal and spatial variations. General increases in surface ozone are calculated for each season, with increases by up to 5% for some regions.


2020 ◽  
Author(s):  
Ewa Bednarz ◽  
Ryan Hossaini ◽  
Luke Abraham ◽  
Martyn Chipperfield

&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.&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. 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. Employing novel estimates of Cl-VSLS emissions we show model results regarding the atmospheric impacts of chlorinated VSLSs over the recent past (2000-present), with a focus on stratospheric ozone and HCl trends. Finally, we introduce our plans regarding examining the impacts of chlorinated VSLSs under a range of potential future emissions scenarios; the results of which will be directly relevant for the next WMO/UNEP assessment.&lt;/p&gt;


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