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93 result(s) for "Krummel, Paul B."
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Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
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.
Role of atmospheric oxidation in recent methane growth
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.
A decline in emissions of CFC-11 and related chemicals from eastern China
Emissions of ozone-depleting substances, including trichlorofluoromethane (CFC-11), have decreased since the mid-1980s in response to the Montreal Protocol 1 , 2 . In recent years, an unexpected increase in CFC-11 emissions beginning in 2013 has been reported, with much of the global rise attributed to emissions from eastern China 3 , 4 . Here we use high-frequency atmospheric mole fraction observations from Gosan, South Korea and Hateruma, Japan, together with atmospheric chemical transport-model simulations, to investigate regional CFC-11 emissions from eastern China. We find that CFC-11 emissions returned to pre-2013 levels in 2019 (5.0 ± 1.0 gigagrams per year in 2019, compared to 7.2 ± 1.5 gigagrams per year for 2008–2012, ±1 standard deviation), decreasing by 10 ± 3 gigagrams per year since 2014–2017. Furthermore, we find that in this region, carbon tetrachloride (CCl 4 ) and dichlorodifluoromethane (CFC-12) emissions—potentially associated with CFC-11 production—were higher than expected after 2013 and then declined one to two years before the CFC-11 emissions reduction. This suggests that CFC-11 production occurred in eastern China after the mandated global phase-out, and that there was a subsequent decline in production during 2017–2018. We estimate that the amount of the CFC-11 bank (the amount of CFC-11 produced, but not yet emitted) in eastern China is up to 112 gigagrams larger in 2019 compared to pre-2013 levels, probably as a result of recent production. Nevertheless, it seems that any substantial delay in ozone-layer recovery has been avoided, perhaps owing to timely reporting 3 , 4 and subsequent action by industry and government in China 5 , 6 . Atmospheric data and chemical-transport modelling show that CFC-11 emissions from eastern China have again decreased, after increasing in 2013–2017, and a delay in ozone-layer recovery has probably been avoided.
Sustained growth of sulfur hexafluoride emissions in China inferred from atmospheric observations
Sulfur hexafluoride (SF 6 ) is a potent greenhouse gas. Here we use long-term atmospheric observations to determine SF 6 emissions from China between 2011 and 2021, which are used to evaluate the Chinese national SF 6 emission inventory and to better understand the global SF 6 budget. SF 6 emissions in China substantially increased from 2.6 (2.3-2.7, 68% uncertainty) Gg yr −1 in 2011 to 5.1 (4.8-5.4) Gg yr −1 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 6 emissions, likely due to substantial power generation and transmission in that area. The CO 2 -eq emissions of SF 6 in China in 2021 were 125 (117-132) million tonnes (Mt), comparable to the national total CO 2 emissions of several countries such as the Netherlands or Nigeria. The increasing SF 6 emissions offset some of the CO 2 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. Atmospheric measurements show that China’s emissions of the potent greenhouse gas, sulfur hexafluoride, grew rapidly between 2011 and 2021. This rise could offset some of China’s progress towards its greenhouse gas emission reduction goal.
Rapid increase in dichloromethane emissions from China inferred through atmospheric observations
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 2 Cl 2 ). The emissions grew from 231 (213–245) Gg yr −1 in 2011 to 628 (599–658) Gg yr −1 in 2019, with an average annual increase of 13 (12–15) %, primarily from eastern China. The overall increase in CH 2 Cl 2 emissions from China has the same magnitude as the global emission rise of 354 (281−427) Gg yr −1 over the same period. If global CH 2 Cl 2 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 2 Cl 2 emissions. Dichloromethane (CH 2 Cl 2 ) is an unregulated ozone depleting substance whose emissions have strongly increased in recent years. Here, the authors show that rising emissions of dichloromethane in China between 2011 and 2019 can explain much of this global increase.
Rapid increase in ozone-depleting chloroform emissions from China
Chloroform contributes to the depletion of the stratospheric ozone layer. However, due to its short lifetime and predominantly natural sources, it is not included in the Montreal Protocol that regulates the production and uses of ozone-depleting substances. Atmospheric chloroform mole fractions were relatively stable or slowly decreased during 1990–2010. Here we show that global chloroform mole fractions increased after 2010, based on in situ chloroform measurements at seven stations around the world. We estimate that the global chloroform emissions grew at the rate of 3.5% yr−1 between 2010 and 2015 based on atmospheric model simulations. We used two regional inverse modelling approaches, combined with observations from East Asia, to show that emissions from eastern China grew by 49 (41–59) Gg between 2010 and 2015, a change that could explain the entire increase in global emissions. We suggest that if chloroform emissions continuously grow at the current rate, the recovery of the stratospheric ozone layer above Antarctica could be delayed by several years.
Atmospheric observations show accurate reporting and little growth in India’s methane emissions
Changes in tropical wetland, ruminant or rice emissions are thought to have played a role in recent variations in atmospheric methane (CH 4 ) concentrations. India has the world’s largest ruminant population and produces ~ 20% of the world’s rice. Therefore, changes in these sources could have significant implications for global warming. Here, we infer India’s CH 4 emissions for the period 2010–2015 using a combination of satellite, surface and aircraft data. We apply a high-resolution atmospheric transport model to simulate data from these platforms to infer fluxes at sub-national scales and to quantify changes in rice emissions. We find that average emissions over this period are 22.0 (19.6–24.3) Tg yr −1 , which is consistent with the emissions reported by India to the United Framework Convention on Climate Change. Annual emissions have not changed significantly (0.2 ± 0.7 Tg yr −1 ) between 2010 and 2015, suggesting that major CH 4 sources did not change appreciably. These findings are in contrast to another major economy, China, which has shown significant growth in recent years due to increasing fossil fuel emissions. However, the trend in a global emission inventory has been overestimated for China due to incorrect rate of fossil fuel growth. Here, we find growth has been overestimated in India but likely due to ruminant and waste sectors. India’s methane emissions have been quantified using atmospheric measurements to provide an independent comparison with reported emissions. Here Ganesan et al. find that derived methane emissions are consistent with India’s reports and no significant trend has been observed between 2010–2015.
Impact of leakage during HFC-125 production on the increase in HCFC-123 and HCFC-124 emissions
Hydrochlorofluorocarbons (HCFCs) are ozone-depleting substances whose production and consumption have been phased out under the Montreal Protocol in non-Article 5 (mainly developed) countries and are currently being phased out in the rest of the world. Here, we focus on two HCFCs, HCFC-123 and HCFC-124, whose emissions are not decreasing globally in line with their phase-out. We present the first measurement-derived estimates of global HCFC-123 emissions (1993–2023) and updated HCFC-124 emissions for 1978–2023. Around 5 Gg yr−1 of HCFC-123 and 3 Gg yr−1 of HCFC-124 were emitted in 2023. Both HCFC-123 and HCFC-124 are intermediates in the production of HFC-125, a non-ozone-depleting hydrofluorocarbon (HFC) that has replaced ozone-depleting substances in many applications. We show that it is possible that the observed global increase in HCFC-124 emissions could be entirely due to leakage from the production of HFC-125, provided that its leakage rate is around 1 % by mass of HFC-125 production. Global emissions of HCFC-123 have not decreased despite its phase-out for production under the Montreal Protocol, and its use in HFC-125 production may be a contributing factor to this. Emissions of HCFC-124 from western Europe, the USA and East Asia have either fallen or not increased since 2015 and together cannot explain the entire increase in the derived global emissions of HCFC-124. These findings add to the growing evidence that emissions of some ozone-depleting substances are increasing due to leakage and improper destruction during fluorochemical production.
Evaluating the contribution of the unexplored photochemistry of aldehydes on the tropospheric levels of molecular hydrogen (H2)
Molecular hydrogen, H2, is one of the most abundant trace gases in the atmosphere. The main known chemical source of H2 in the atmosphere is the photolysis of formaldehyde and glyoxal. Recent laboratory measurements and ground-state photochemistry calculations have shown other aldehydes photodissociate to yield H2 as well. This aldehyde photochemistry has not been previously accounted for in atmospheric H2 models. Here, we used two atmospheric models to test the implications of the previously unexplored aldehyde photochemistry on the H2 tropospheric budget. We used the AtChem box model implementing the nearly chemically explicit Master Chemical Mechanism at three sites selected to represent variable atmospheric environments: London, Cabo Verde and Borneo. We conducted five box model simulations per site using varying quantum yields for the photolysis of 16 aldehydes and compared the results against a baseline. The box model simulations showed that the photolysis of acetaldehyde, propanal, methylglyoxal, glycolaldehyde and methacrolein yields the highest chemical production of H2. We also used the GEOS-Chem 3-D atmospheric chemical transport model to test the impacts of the new photolytic H2 source on the global scale. A new H2 simulation capability was developed in GEOS-Chem and evaluated for 2015 and 2016. We then performed a sensitivity simulation in which the photolysis reactions of six aldehyde species were modified to include a 1 % yield of H2. We found an increase in the chemical production of H2 over tropical regions where high abundance of isoprene results in the secondary generation of methylglyoxal, glycolaldehyde and methacrolein, ultimately yielding H2. We calculated a final increase of 0.4 Tg yr−1 in the global chemical production budget, compared to a baseline production of ∼41 Tg yr−1. Ultimately, both models showed that H2 production from the newly discovered photolysis of aldehydes leads to only minor changes in the atmospheric mixing ratios of H2, at least for the aldehydes tested here when assuming a 1 % quantum yield across all wavelengths. Our results imply that the previously missing photochemical source is a less significant source of model uncertainty than other components of the H2 budget, including emissions and soil uptake.
Global emissions of perfluorocyclobutane (PFC-318, c -C 4 F 8 ) resulting from the use of hydrochlorofluorocarbon-22 (HCFC-22) feedstock to produce polytetrafluoroethylene (PTFE) and related fluorochemicals
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.