Role of atmospheric oxidation in recent methane growth Rigby, Matthew; Montzka, Stephen A.; Prinn, Ronald G. ...
Proceedings of the National Academy of Sciences - PNAS,
05/2017, Letnik:
114, Številka:
21
Journal Article
Recenzirano
Odprti dostop
The growth in global methane (CH₄) concentration, which had been ongoing since the industrial revolution, stalled around the year 2000 before resuming globally in 2007. We evaluate the role of the ...hydroxyl radical (OH), the major CH₄ sink, in the recent CH₄ growth. We also examine the influence of systematic uncertainties in OH concentrations on CH₄ emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH₃CCl₃), which is lost primarily through reaction with OH, to estimate OH levels as well as CH₃CCl₃ emissions, which have uncertainty that previously limited the accuracy of OH estimates. We find a 64–70% probability that a decline in OH has contributed to the post-2007 methane rise. Our median solution suggests that CH₄ emissions increased relatively steadily during the late 1990s and early 2000s, after which growth was more modest. This solution obviates the need for a sudden statistically significant change in total CH₄ emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13CH₄/12CH₄ ratio and the recent growth in C₂H₆. Our approach indicates that significant OH-related uncertainties in the CH₄ budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH₄ emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered.
With the successful implementation of the Montreal Protocol on Substances that Deplete the Ozone Layer, the atmospheric abundance of ozone-depleting substances continues to decrease slowly and the ...Antarctic ozone hole is showing signs of recovery. However, growing emissions of unregulated short-lived anthropogenic chlorocarbons are offsetting some of these gains. Here, we report an increase in emissions from China of the industrially produced chlorocarbon, dichloromethane (CH
Cl
). The emissions grew from 231 (213-245) Gg yr
in 2011 to 628 (599-658) Gg yr
in 2019, with an average annual increase of 13 (12-15) %, primarily from eastern China. The overall increase in CH
Cl
emissions from China has the same magnitude as the global emission rise of 354 (281-427) Gg yr
over the same period. If global CH
Cl
emissions remain at 2019 levels, they could lead to a delay in Antarctic ozone recovery of around 5 years compared to a scenario with no CH
Cl
emissions.
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.
Sulfur hexafluoride (SF
) is a potent greenhouse gas. Here we use long-term atmospheric observations to determine SF
emissions from China between 2011 and 2021, which are used to evaluate the Chinese ...national SF
emission inventory and to better understand the global SF
budget. SF
emissions in China substantially increased from 2.6 (2.3-2.7, 68% uncertainty) Gg yr
in 2011 to 5.1 (4.8-5.4) Gg yr
in 2021. The increase from China is larger than the global total emissions rise, implying that it has offset falling emissions from other countries. Emissions in the less-populated western regions of China, which have potentially not been well quantified in previous measurement-based estimates, contribute significantly to the national SF
emissions, likely due to substantial power generation and transmission in that area. The CO
-eq emissions of SF
in China in 2021 were 125 (117-132) million tonnes (Mt), comparable to the national total CO
emissions of several countries such as the Netherlands or Nigeria. The increasing SF
emissions offset some of the CO
reductions achieved through transitioning to renewable energy in the power industry, and might hinder progress towards achieving China's goal of carbon neutrality by 2060 if no concrete control measures are implemented.
The reaction of CH _4 with chlorine (Cl) radicals in the atmosphere is associated with an extraordinarily strong isotopic fractionation, where ^12 CH _4 reacts about 70 ‰ faster with Cl than ^13 CH ..._4 . Therefore, although the Cl-based sink of CH _4 constitutes only a small contribution to its total removal rate, the uncertainty in this small sink has been identified as one of the two largest uncertainties of isotope-based CH _4 source apportionment at the global scale. The uncertainty arises from the fact that Cl levels in the atmosphere are so low that they cannot be detected directly. One very sensitive indirect method to identify and quantify the CH _4 + Cl reaction in the atmosphere is the detection of the extremely ^13 C-depleted reaction product carbon monoxide (CO) from this reaction. This article reviews the concept of this approach, its successful application in the atmosphere, its challenges and opportunities for identifying and quantifying Cl-based removal of CH _4 at the regional and global scale and its potential to detect and evaluate possible attempts to enhance CH _4 removal from the atmosphere.
We infer global and regional emissions of five of the most abundant hydrofluorocarbons (HFCs) using atmospheric measurements from the Advanced Global Atmospheric Gases Experiment and the National ...Institute for Environmental Studies, Japan, networks. We find that the total CO₂-equivalent emissions of the five HFCs from countries that are required to provide detailed, annual reports to the United Nations Framework Convention on Climate Change (UNFCCC) increased from 198 (175–221) Tg-CO₂-eq·y⁻¹ in 2007 to 275 (246–304) Tg-CO₂-eq·y⁻¹ in 2012. These global warming potential-weighted aggregated emissions agree well with those reported to the UNFCCC throughout this period and indicate that the gap between reported emissions and global HFC emissions derived from atmospheric trends is almost entirely due to emissions from nonreporting countries. However, our measurement-based estimates of individual HFC species suggest that emissions, from reporting countries, of the most abundant HFC, HFC-134a, were only 79% (63–95%) of the UNFCCC inventory total, while other HFC emissions were significantly greater than the reported values. These results suggest that there are inaccuracies in the reporting methods for individual HFCs, which appear to cancel when aggregated together.
Very short‐lived substances (VSLS), including dichloromethane (CH2Cl2), chloroform (CHCl3), perchloroethylene (C2Cl4), and 1,2‐dichloroethane (C2H4Cl2), are a stratospheric chlorine source and ...therefore contribute to ozone depletion. We quantify stratospheric chlorine trends from these VSLS (VSLCltot) using a chemical transport model and atmospheric measurements, including novel high‐altitude aircraft data from the NASA VIRGAS (2015) and POSIDON (2016) missions. We estimate VSLCltot increased from 69 (±14) parts per trillion (ppt) Cl in 2000 to 111 (±22) ppt Cl in 2017, with >80% delivered to the stratosphere through source gas injection, and the remainder from product gases. The modeled evolution of chlorine source gas injection agrees well with historical aircraft data, which corroborate reported surface CH2Cl2 increases since the mid‐2000s. The relative contribution of VSLS to total stratospheric chlorine increased from ~2% in 2000 to ~3.4% in 2017, reflecting both VSLS growth and decreases in long‐lived halocarbons. We derive a mean VSLCltot growth rate of 3.8 (±0.3) ppt Cl/year between 2004 and 2017, though year‐to‐year growth rates are variable and were small or negative in the period 2015–2017. Whether this is a transient effect, or longer‐term stabilization, requires monitoring. In the upper stratosphere, the modeled rate of HCl decline (2004–2017) is −5.2% per decade with VSLS included, in good agreement to ACE satellite data (−4.8% per decade), and 15% slower than a model simulation without VSLS. Thus, VSLS have offset a portion of stratospheric chlorine reductions since the mid‐2000s.
Plain Language Summary
It is well established that long‐lived halogen‐containing compounds of anthropogenic origin, such as chlorofluorocarbons, have led to depletion of the stratospheric ozone layer. As production of these compounds is now controlled by the Montreal Protocol, the atmospheric abundance of chlorine/bromine is in decline, and the ozone layer should “recover” in coming decades. Here we consider the contribution of Very Short‐Lived Substances to stratospheric chlorine. These compounds also have anthropogenic sources, though are much less efficient at destroying ozone compared to, for example, most chlorofluorocarbons (per molecule emitted) as they break down more readily close to Earth's surface. Using surface observations and atmospheric model simulations, we show that stratospheric chlorine from short‐lived substances has increased since the early 2000s. This increase is also apparent from airborne measurements of their atmospheric abundance over the same period. Using the model in conjunction with satellite estimates of stratospheric chlorine, we show rising levels of short‐lived substances may be causing upper stratospheric chlorine to decline at a slower rate relative to what would be expected in their absence. While this offset in the rate of chlorine decline is modest (15%), it is nonnegligible and should be considered in the analysis of stratospheric composition trends.
Key Points
Stratospheric chlorine from very short‐lived substances increased by 3.8 ppt/year over 2004–2017, with a growth slowdown in 2015–2017
Chlorine from short‐lived substances improves model representation of upper stratospheric HCl trends
Short‐lived chlorine offsets the 2004–2017 rate of upper stratospheric HCl decline by 15%
We present top-down constraints on global monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an ...array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies include (1) a standard 4D-Var inversion at native model resolution (4° × 5°), (2) an inversion for six continental and three ocean regions, and (3) a fast 4D-Var inversion based on a novel dimension reduction technique employing randomized singular value decomposition (SVD). The optimized global flux ranges from 15.9 Tg N yr−1 (SVD-based inversion) to 17.5–17.7 Tg N yr−1 (continental-scale, standard 4D-Var inversions), with the former better capturing the extratropical N2O background measured during the HIAPER Pole-to-Pole Observations (HIPPO) airborne campaigns. We find that the tropics provide a greater contribution to the global N2O flux than is predicted by the prior bottom-up inventories, likely due to underestimated agricultural and oceanic emissions. We infer an overestimate of natural soil emissions in the extratropics and find that predicted emissions are seasonally biased in northern midlatitudes. Here, optimized fluxes exhibit a springtime peak consistent with the timing of spring fertilizer and manure application, soil thawing, and elevated soil moisture. Finally, the inversions reveal a major emission underestimate in the US Corn Belt in the bottom-up inventory used here. We extensively test the impact of initial conditions on the analysis and recommend formally optimizing the initial N2O distribution to avoid biasing the inferred fluxes. We find that the SVD-based approach provides a powerful framework for deriving emission information from N2O observations: by defining the optimal resolution of the solution based on the information content of the inversion, it provides spatial information that is lost when aggregating to political or geographic regions, while also providing more temporal information than a standard 4D-Var inversion.
The growth in atmospheric methane (CH4) concentrations over the past 2 decades has shown large variability on a timescale of several years. Prior to 1999 the globally averaged CH4 concentration was ...increasing at a rate of 6.0 ppb yr−1, but during a stagnation period from 1999 to 2006 this growth rate slowed to 0.6 ppb yr−1. From 2007 to 2009 the growth rate again increased to 4.9 ppb yr−1. These changes in growth rate are usually ascribed to variations in CH4 emissions. We have used a 3-D global chemical transport model, driven by meteorological reanalyses and variations in global mean hydroxyl (OH) concentrations derived from CH3CCl3 observations from two independent networks, to investigate these CH4 growth variations. The model shows that between 1999 and 2006 changes in the CH4 atmospheric loss contributed significantly to the suppression in global CH4 concentrations relative to the pre-1999 trend. The largest factor in this is relatively small variations in global mean OH on a timescale of a few years, with minor contributions of atmospheric transport of CH4 to its sink region and of atmospheric temperature. Although changes in emissions may be important during the stagnation period, these results imply a smaller variation is required to explain the observed CH4 trends. The contribution of OH variations to the renewed CH4 growth after 2007 cannot be determined with data currently available.
The atmospheric concentration of trichlorofluoromethane (CFC-11) has been in decline since the production of ozone-depleting substances was phased out under the Montreal Protocol
. Since 2013, the ...concentration decline of CFC-11 slowed unexpectedly owing to increasing emissions, probably from unreported production, which, if sustained, would delay the recovery of the stratospheric ozone layer
. Here we report an accelerated decline in the global mean CFC-11 concentration during 2019 and 2020, derived from atmospheric concentration measurements at remote sites around the world. We find that global CFC-11 emissions decreased by 18 ± 6 gigagrams per year (26 ± 9 per cent; one standard deviation) from 2018 to 2019, to a 2019 value (52 ± 10 gigagrams per year) that is similar to the 2008-2012 mean. The decline in global emissions suggests a substantial decrease in unreported CFC-11 production. If the sharp decline in unexpected global emissions and unreported production is sustained, any associated future ozone depletion is likely to be limited, despite an increase in the CFC-11 bank (the amount of CFC-11 produced, but not yet emitted) by 90 to 725 gigagrams by the beginning of 2020.
PDF
