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Showing papers on "Atmospheric methane published in 2016"


Journal ArticleDOI
10 Mar 2016-Nature
TL;DR: The cumulative warming capacity of concurrent biogenic methane and nitrous oxide emissions is a factor of about two larger than the cooling effect resulting from the global land carbon dioxide uptake from 2001 to 2010, which results in a net positive cumulative impact of the three greenhouse gases on the planetary energy budget.
Abstract: The net balance of terrestrial biogenic greenhouse gases produced as a result of human activities and the climatic impact of this balance are uncertain; here the net cumulative impact of the three greenhouse gases, methane, nitrous oxide and carbon dioxide, on the planetary energy budget from 2001 to 2010 is a warming of the planet. The biogenic fluxes of individual greenhouse gases have extensively studied, but the net terrestrial biogenic greenhouse gas balance as a result of human activities and its climatic impact remains uncertain. Hanqin Tian et al. have quantified the net cumulative impact of three greenhouse gases — methane, nitrous oxide and carbon dioxide — on the planetary energy budget. From 2001 to 2010, they find a net positive (warming) cumulative impact and conclude that a reduction in agricultural methane and nitrous oxide emissions — in particular in Southern Asia — may help mitigate climate change. The terrestrial biosphere can release or absorb the greenhouse gases, carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O), and therefore has an important role in regulating atmospheric composition and climate1. Anthropogenic activities such as land-use change, agriculture and waste management have altered terrestrial biogenic greenhouse gas fluxes, and the resulting increases in methane and nitrous oxide emissions in particular can contribute to climate change2,3. The terrestrial biogenic fluxes of individual greenhouse gases have been studied extensively4,5,6, but the net biogenic greenhouse gas balance resulting from anthropogenic activities and its effect on the climate system remains uncertain. Here we use bottom-up (inventory, statistical extrapolation of local flux measurements, and process-based modelling) and top-down (atmospheric inversions) approaches to quantify the global net biogenic greenhouse gas balance between 1981 and 2010 resulting from anthropogenic activities and its effect on the climate system. We find that the cumulative warming capacity of concurrent biogenic methane and nitrous oxide emissions is a factor of about two larger than the cooling effect resulting from the global land carbon dioxide uptake from 2001 to 2010. This results in a net positive cumulative impact of the three greenhouse gases on the planetary energy budget, with a best estimate (in petagrams of CO2 equivalent per year) of 3.9 ± 3.8 (top down) and 5.4 ± 4.8 (bottom up) based on the GWP100 metric (global warming potential on a 100-year time horizon). Our findings suggest that a reduction in agricultural methane and nitrous oxide emissions, particularly in Southern Asia, may help mitigate climate change.

398 citations


Journal ArticleDOI
06 Oct 2016-Nature
TL;DR: The largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources, finds that total fossil fuel methane emissions are not increasing over time, but are 60 to 110 per cent greater than current estimates owing to large revisions in isotope source signatures.
Abstract: Revisions in isotopic source signatures reveal that global total fossil fuel methane emissions from industry plus natural geological seepage are much larger than thought. Stefan Schwietzke et al. re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions on the basis of long-term global methane and methane carbon isotope records. They find that total fossil fuel methane emissions (fossil fuel industry plus natural geological methane seepage) are not increasing over time, but are 60–110 per cent greater than was previously thought. They also conclude that methane emissions from natural gas, oil and coal production and their usage are 20–60 per cent greater than inventories and that methane emissions from natural gas as a fraction of production have declined from about 8 per cent to 2 per cent over the past three decades. Methane has the second-largest global radiative forcing impact of anthropogenic greenhouse gases after carbon dioxide, but our understanding of the global atmospheric methane budget is incomplete. The global fossil fuel industry (production and usage of natural gas, oil and coal) is thought to contribute 15 to 22 per cent of methane emissions1,2,3,4,5,6,7,8,9,10 to the total atmospheric methane budget11. However, questions remain regarding methane emission trends as a result of fossil fuel industrial activity and the contribution to total methane emissions of sources from the fossil fuel industry and from natural geological seepage12,13, which are often co-located. Here we re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions based on long-term global methane and methane carbon isotope records. We compile the largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources. We find that total fossil fuel methane emissions (fossil fuel industry plus natural geological seepage) are not increasing over time, but are 60 to 110 per cent greater than current estimates1,2,3,4,5,6,7,8,9,10 owing to large revisions in isotope source signatures. We show that this is consistent with the observed global latitudinal methane gradient. After accounting for natural geological methane seepage12,13, we find that methane emissions from natural gas, oil and coal production and their usage are 20 to 60 per cent greater than inventories1,2. Our findings imply a greater potential for the fossil fuel industry to mitigate anthropogenic climate forcing, but we also find that methane emissions from natural gas as a fraction of production have declined from approximately 8 per cent to approximately 2 per cent over the past three decades.

374 citations


Journal ArticleDOI
01 Apr 2016-Science
TL;DR: The atmospheric methane level has resumed its increase after a plateau between 1999 and 2006, and a box-model analysis suggests that diminishing thermogenic emissions, probably from the fossil-fuel industry, and/or variations in the hydroxyl CH4 sink caused the plateau.
Abstract: Between 1999 and 2006, a plateau interrupted the otherwise continuous increase of atmospheric methane concentration [CH4] since preindustrial times. Causes could be sink variability or a temporary reduction in industrial or climate-sensitive sources. We reconstructed the global history of [CH4] and its stable carbon isotopes from ice cores, archived air, and a global network of monitoring stations. A box-model analysis suggests that diminishing thermogenic emissions, probably from the fossil-fuel industry, and/or variations in the hydroxyl CH4 sink caused the [CH4] plateau. Thermogenic emissions did not resume to cause the renewed [CH4] rise after 2006, which contradicts emission inventories. Post-2006 source increases are predominantly biogenic, outside the Arctic, and arguably more consistent with agriculture than wetlands. If so, mitigating CH4 emissions must be balanced with the need for food production.

316 citations


Journal ArticleDOI
TL;DR: The isotopic evidence presented in this article suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies.
Abstract: From 2007 to 2013, the globally averaged mole fraction of methane in the atmosphere increased by 5.7 ± 1.2 ppb yr−1. Simultaneously, δ13CCH4 (a measure of the 13C/12C isotope ratio in methane) has shifted to significantly more negative values since 2007. Growth was extreme in 2014, at 12.5 ± 0.4 ppb, with a further shift to more negative values being observed at most latitudes. The isotopic evidence presented here suggests that the methane rise was dominated by significant increases in biogenic methane emissions, particularly in the tropics, for example, from expansion of tropical wetlands in years with strongly positive rainfall anomalies or emissions from increased agricultural sources such as ruminants and rice paddies. Changes in the removal rate of methane by the OH radical have not been seen in other tracers of atmospheric chemistry and do not appear to explain short-term variations in methane. Fossil fuel emissions may also have grown, but the sustained shift to more 13C-depleted values and its significant interannual variability, and the tropical and Southern Hemisphere loci of post-2007 growth, both indicate that fossil fuel emissions have not been the dominant factor driving the increase. A major cause of increased tropical wetland and tropical agricultural methane emissions, the likely major contributors to growth, may be their responses to meteorological change.

293 citations


Journal ArticleDOI
TL;DR: It is shown that when the particle size of zinc oxide is reduced down to the nanoscale, it exhibits high activity for methane oxidation under simulated sunlight illumination, and nano silver decoration further enhances the photo-activity via the surface plasmon resonance.
Abstract: The search for active catalysts that efficiently oxidize methane under ambient conditions remains a challenging task for both C1 utilization and atmospheric cleansing. Here, we show that when the particle size of zinc oxide is reduced down to the nanoscale, it exhibits high activity for methane oxidation under simulated sunlight illumination, and nano silver decoration further enhances the photo-activity via the surface plasmon resonance. The high quantum yield of 8% at wavelengths <400 nm and over 0.1% at wavelengths ∼470 nm achieved on the silver decorated zinc oxide nanostructures shows great promise for atmospheric methane oxidation. Moreover, the nano-particulate composites can efficiently photo-oxidize other small molecular hydrocarbons such as ethane, propane and ethylene, and in particular, can dehydrogenize methane to generate ethane, ethylene and so on. On the basis of the experimental results, a two-step photocatalytic reaction process is suggested to account for the methane photo-oxidation.

283 citations


Journal ArticleDOI
TL;DR: The recent rapid rise in global methane concentrations is predominantly biogenic-most likely from agriculture-with smaller contributions from fossil fuel use and possibly wetlands as discussed by the authors, but the reasons for this renewed growth are still unclear, primarily because of uncertainties in the global methane budget.
Abstract: Unlike CO2, atmospheric methane concentrations are rising faster than at any time in the past two decades and, since 2014, are now approaching the most greenhouse-gas-intensive scenarios. The reasons for this renewed growth are still unclear, primarily because of uncertainties in the global methane budget. New analysis suggests that the recent rapid rise in global methane concentrations is predominantly biogenic-most likely from agriculture-with smaller contributions from fossil fuel use and possibly wetlands. Additional attention is urgently needed to quantify and reduce methane emissions. Methane mitigation offers rapid climate benefits and economic, health and agricultural co-benefits that are highly complementary to CO2 mitigation.

264 citations


Journal ArticleDOI
TL;DR: In this paper, the authors review the value of current, future, and proposed satellite observations to better quantify and understand methane emissions through inverse analyses, from the global scale down to the scale of point sources and in combination with suborbital (surface and aircraft) data.
Abstract: . Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned for launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify and understand methane emissions through inverse analyses, from the global scale down to the scale of point sources and in combination with suborbital (surface and aircraft) data. Current global observations from Greenhouse Gases Observing Satellite (GOSAT) are of high quality but have sparse spatial coverage. They can quantify methane emissions on a regional scale (100–1000 km) through multiyear averaging. The Tropospheric Monitoring Instrument (TROPOMI), to be launched in 2017, is expected to quantify daily emissions on the regional scale and will also effectively detect large point sources. A different observing strategy by GHGSat (launched in June 2016) is to target limited viewing domains with very fine pixel resolution in order to detect a wide range of methane point sources. Geostationary observation of methane, still in the proposal stage, will have the unique capability of mapping source regions with high resolution, detecting transient "super-emitter" point sources and resolving diurnal variation of emissions from sources such as wetlands and manure. Exploiting these rapidly expanding satellite measurement capabilities to quantify methane emissions requires a parallel effort to construct high-quality spatially and sectorally resolved emission inventories. Partnership between top-down inverse analyses of atmospheric data and bottom-up construction of emission inventories is crucial to better understanding methane emission processes and subsequently informing climate policy.

213 citations


Journal ArticleDOI
TL;DR: This paper used nuclear magnetic resonance spectroscopy to show that polysaccharide esters of three phosphonic acids are important constituents of dissolved organic matter in seawater from the North Pacific.
Abstract: A lot of methane is emitted from oxygenated seawater, where its production should be inhibited. Seawater incubations and organic matter characterizations reveal that bacteria aerobically produce methane from phosphonates in organic matter. Biogenic methane is widely thought to be a product of archaeal methanogenesis, an anaerobic process that is inhibited or outcompeted by the presence of oxygen and sulfate1,2,3. Yet a large fraction of marine methane delivered to the atmosphere is produced in high-sulfate, fully oxygenated surface waters that have methane concentrations above atmospheric equilibrium values, an unexplained phenomenon referred to as the marine methane paradox4,5. Here we use nuclear magnetic resonance spectroscopy to show that polysaccharide esters of three phosphonic acids are important constituents of dissolved organic matter in seawater from the North Pacific. In seawater and pure culture incubations, bacterial degradation of these dissolved organic matter phosphonates in the presence of oxygen releases methane, ethylene and propylene gas. Moreover, we found that in mutants of a methane-producing marine bacterium, Pseudomonas stutzeri, disrupted in the C–P lyase phosphonate degradation pathway, methanogenesis was also disabled, indicating that the C–P lyase pathway can catalyse methane production from marine dissolved organic matter. Finally, the carbon stable isotope ratio of methane emitted during our incubations agrees well with anomalous isotopic characteristics of seawater methane. We estimate that daily cycling of only about 0.25% of the organic matter phosphonate inventory would support the entire atmospheric methane flux at our study site. We conclude that aerobic bacterial degradation of phosphonate esters in dissolved organic matter may explain the marine methane paradox.

212 citations


Journal ArticleDOI
TL;DR: The induction of HAMO activity occurred only after the rapid growth of methanotrophic populations, and a metatranscriptome-wide association study suggests that the concurrent high- and low-affinity methane oxidation was catalysed by known meethanotrophs rather than by the proposed novel atmospheric methane oxidizers.
Abstract: Soils serve as the biological sink of the potent greenhouse gas methane with exceptionally low concentrations of ∼1.84 p.p.m.v. in the atmosphere. The as-yet-uncultivated methane-consuming bacteria have long been proposed to be responsible for this 'high-affinity' methane oxidation (HAMO). Here we show an emerging HAMO activity arising from conventional methanotrophs in paddy soil. HAMO activity was quickly induced during the low-affinity oxidation of high-concentration methane. Activity was lost gradually over 2 weeks, but could be repeatedly regained by flush-feeding the soil with elevated methane. The induction of HAMO activity occurred only after the rapid growth of methanotrophic populations, and a metatranscriptome-wide association study suggests that the concurrent high- and low-affinity methane oxidation was catalysed by known methanotrophs rather than by the proposed novel atmospheric methane oxidizers. These results provide evidence of atmospheric methane uptake in periodically drained ecosystems that are typically considered to be a source of atmospheric methane.

183 citations


Journal ArticleDOI
TL;DR: An overview of recent literature that focuses on conversion of methane to methanol, with a focus primarily on the manufacturing systems and processes used in this conversion, can be found in this paper.
Abstract: The emission of greenhouse gases (GHGs) is a major air pollution issue that affects climate change across the globe. Methane (CH 4 ), behind carbon dioxide (CO 2 ), is the second most abundant GHGs that negatively impact the atmosphere layer. Many studies have been conducted to identify a method for reducing the concentration of methane in the atmosphere. Converting methane to alternative forms source of energy, such as methanol, is a preferred method for methane reduction. This review aims to present an overview of recent literature that focuses on conversion of methane to methanol, with a focus primarily on the manufacturing systems and processes used in this conversion. Basic descriptions are given of several relevant technologies for converting methane to methanol and their characteristics, including conventional catalytic processes, plasma technology, photo-catalysts, supercritical water processes, biological processes and other processes. All of these options are feasible for use in the conversion process of methane to methanol.

180 citations


Journal ArticleDOI
TL;DR: In this paper, the authors quantified the magnitude of the second class of sources, using long-term measurements of atmospheric ethane as a tracer for thermogenic methane emissions.
Abstract: . Harmonized time series of column-averaged mole fractions of atmospheric methane and ethane over the period 1999–2014 are derived from solar Fourier transform infrared (FTIR) measurements at the Zugspitze summit (47° N, 11° E; 2964 m a.s.l.) and at Lauder (45° S, 170° E; 370 m a.s.l.). Long-term trend analysis reveals a consistent renewed methane increase since 2007 of 6.2 [5.6, 6.9] ppb yr−1 (parts-per-billion per year) at the Zugspitze and 6.0 [5.3, 6.7] ppb yr−1 at Lauder (95 % confidence intervals). Several recent studies provide pieces of evidence that the renewed methane increase is most likely driven by two main factors: (i) increased methane emissions from tropical wetlands, followed by (ii) increased thermogenic methane emissions due to growing oil and natural gas production. Here, we quantify the magnitude of the second class of sources, using long-term measurements of atmospheric ethane as a tracer for thermogenic methane emissions. In 2007, after years of weak decline, the Zugspitze ethane time series shows the sudden onset of a significant positive trend (2.3 [1.8, 2.8] × 10−2 ppb yr−1 for 2007–2014), while a negative trend persists at Lauder after 2007 (−0.4 [−0.6, −0.1] × 10−2 ppb yr−1). Zugspitze methane and ethane time series are significantly correlated for the period 2007–2014 and can be assigned to thermogenic methane emissions with an ethane-to-methane ratio (EMR) of 12–19 %. We present optimized emission scenarios for 2007–2014 derived from an atmospheric two-box model. From our trend observations we infer a total ethane emission increase over the period 2007–2014 from oil and natural gas sources of 1–11 Tg yr−1 along with an overall methane emission increase of 24–45 Tg yr−1. Based on these results, the oil and natural gas emission contribution (C) to the renewed methane increase is deduced using three different emission scenarios with dedicated EMR ranges. Reference scenario 1 assumes an oil and gas emission combination with EMR = 7.0–16.2 %, which results in a minimum contribution C > 39 % (given as lower bound of 95 % confidence interval). Beside this most plausible scenario 1, we consider two less realistic limiting cases of pure oil-related emissions (scenario 2 with EMR = 16.2–31.4 %) and pure natural gas sources (scenario 3 with EMR = 4.4–7.0 %), which result in C > 18 % and C > 73 %, respectively. Our results suggest that long-term observations of column-averaged ethane provide a valuable constraint on the source attribution of methane emission changes and provide basic knowledge for developing effective climate change mitigation strategies.

Journal ArticleDOI
TL;DR: The spatial distribution of emissions has a dominant effect on global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from the tropics and subtropics.
Abstract: Ozone is an air pollutant and a greenhouse gas. Simulations with a global chemistry transport model reveal that the spatial distribution of ozone precursor emissions dominates the global ozone burden, and that emissions in the tropics matter most. Ozone is an important air pollutant at the surface1, and the third most important anthropogenic greenhouse gas in the troposphere2. Since 1980, anthropogenic emissions of ozone precursors—methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx)—have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards3,4,5,6, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity7,8,9,10,11. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Journal ArticleDOI
TL;DR: The relationships between lake productivity, methanogenesis, and depth-dependent ebullition suggests it is likely that shallow, productive lakes contribute significantly more methane to the atmosphere than deep, clear lakes and will continue to do so in light of the growing prevalence of lake eutrophication.
Abstract: Despite significant contributions of inland lakes to the global methane cycle, we lack a process-based understanding of what regulates inter-lake variation in methane emissions. Previous comparative work has identified a potential link between lake primary productivity and methane emissions; also, lab-scale experiments suggest that the addition of algal substrate to anoxic sediments rapidly enhances rates of methanogenesis. This existing work indicates that primary productivity could enhance lake contributions to the global methane cycle. However, a more systematic investigation of the links between lake primary production, methanogenesis, and methane emission to the atmosphere is required to quantify the implications of increased cultural eutrophication for methane evasion from lakes. Using paired measurements of methanogenesis and methane emissions on 16 north temperate lakes, we documented a positive relationship between lake productivity and sediment methanogenesis rates. However, increased methanogenesis rates did not result in an increase in diffusive methane emissions. Rather, they generated greater methane storage during summer stratification and enhanced methane emission to the atmosphere via bubbling (ebullition), dependent on site depth. Ebullition most frequently occurred at sites less than 6 m deep and where methanogenesis rates were high. The relationships between lake productivity, methanogenesis, and depth-dependent ebullition suggests it is likely that shallow, productive lakes contribute significantly more methane to the atmosphere than deep, clear lakes and will continue to do so in light of the growing prevalence of lake eutrophication.

Journal ArticleDOI
TL;DR: In this article, the authors used satellite retrievals and surface observations of atmospheric methane to suggest that U.S. anthropogenic methane emissions have increased by more than 30% over the 2002-2014 period.
Abstract: The global burden of atmospheric methane has been increasing over the past decade, but the causes are not well understood. National inventory estimates from the U.S. Environmental Protection Agency indicate no significant trend in U.S. anthropogenic methane emissions from 2002 to present. Here we use satellite retrievals and surface observations of atmospheric methane to suggest that U.S. methane emissions have increased by more than 30% over the 2002–2014 period. The trend is largest in the central part of the country, but we cannot readily attribute it to any specific source type. This large increase in U.S. methane emissions could account for 30–60% of the global growth of atmospheric methane seen in the past decade.

Journal ArticleDOI
TL;DR: To fully evaluate the net effect of management practice on the greenhouse gas balance from high latitude peatlands, both net ecosystem exchange (NEE) and carbon exports need to be considered.
Abstract: Northern peatlands constitute a significant source of atmospheric methane (CH4). However, management of undisturbed peatlands, as well as the restoration of disturbed peatlands, will alter the exchange of CH4 with the atmosphere. The aim of this systematic review and meta-analysis was to collate and analyze published studies to improve our understanding of the factors that control CH4 emissions and the impacts of management on the gas flux from northern (latitude 40° to 70°N) peatlands. The analysis includes a total of 87 studies reporting measurements of CH4 emissions taken at 186 sites covering different countries, peatland types, and management systems. Results show that CH4 emissions from natural northern peatlands are highly variable with a 95% CI of 7.6–15.7 g C m−2 year−1 for the mean and 3.3–6.3 g C m−2 year−1 for the median. The overall annual average (mean ± SD) is 12 ± 21 g C m−2 year−1 with the highest emissions from fen ecosystems. Methane emissions from natural peatlands are mainly controlled by water table (WT) depth, plant community composition, and soil pH. Although mean annual air temperature is not a good predictor of CH4 emissions by itself, the interaction between temperature, plant community cover, WT depth, and soil pH is important. According to short-term forecasts of climate change, these complex interactions will be the main determinant of CH4 emissions from northern peatlands. Drainage significantly (p < .05) reduces CH4 emissions to the atmosphere, on average by 84%. Restoration of drained peatlands by rewetting or vegetation/rewetting increases CH4 emissions on average by 46% compared to the original premanagement CH4 fluxes. However, to fully evaluate the net effect of management practice on the greenhouse gas balance from high latitude peatlands, both net ecosystem exchange (NEE) and carbon exports need to be considered.

Journal ArticleDOI
TL;DR: In this paper, the principal physical and biogeochemical processes that regulate methane fluxes across the seabed, the fate of this methane in the water column, and potential for its release to the atmosphere are reviewed.
Abstract: Large quantities of methane are stored in hydrates and permafrost within shallow marine sediments in the Arctic Ocean. These reservoirs are highly sensitive to climate warming, but the fate of methane released from sediments is uncertain. Here, we review the principal physical and biogeochemical processes that regulate methane fluxes across the seabed, the fate of this methane in the water column, and potential for its release to the atmosphere. We find that, at present, fluxes of dissolved methane are significantly moderated by anaerobic and aerobic oxidation of methane. If methane fluxes increase then a greater proportion of methane will be transported by advection or in the gas phase, which reduces the efficiency of the methanotrophic sink. Higher freshwater discharge to Arctic shelf seas may increase stratification and inhibit transfer of methane gas to surface waters, although there is some evidence that increased stratification may lead to warming of sub-pycnocline waters, increasing the potential for hydrate dissociation. Loss of sea-ice is likely to increase wind speeds and sea-air exchange of methane will consequently increase. Studies of the distribution and cycling of methane beneath and within sea ice are limited, but it seems likely that the sea-air methane flux is higher during melting in seasonally ice-covered regions. Our review reveals that increased observations around especially the anaerobic and aerobic oxidation of methane, bubble transport, and the effects of ice cover, are required to fully understand the linkages and feedback pathways between climate warming and release of methane from marine sediments.

Journal ArticleDOI
TL;DR: In this paper, the authors used time series of C2H6 total columns derived from ground-based Fourier transform infrared (FTIR) observations made at five selected Network for theDetection of Atmospheric CompositionChange sites to characterize the recent C 2H6 evolution and determine growth rates of∼5% yr at mid-latitudes and of ∼3% at remote sites.
Abstract: Sharp rises in the atmospheric abundance of ethane (C2H6)have been detected from2009 onwards in theNorthernHemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs inNorthAmerica. Using time series of C2H6 total columns derived from groundbased Fourier transform infrared (FTIR) observationsmade atfive selectedNetwork for theDetection of Atmospheric CompositionChange sites, we characterize the recent C2H6 evolution and determine growth rates of∼5% yr atmid-latitudes and of∼3% yr at remote sites. Results fromCAM-chem simulations with theHemispheric Transport of Air Pollutants, Phase II bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009.We further estimate thatNorthAmerican anthropogenic C2H6 emissions have increased from1.6 Tg yr −1 in 2008 to 2.8 Tg yr in 2014, i.e. by 75%over these six years.We also completed a second simulation with new top-down emissions of C2H6 fromNorthAmerican oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations ofmethane (CH4) from GreenhouseGasesObserving SATellite. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at themid-latitudinal sites, underscoring the impact of theNorthAmerican oil and gas development on the current C2H6 abundance. Finally we estimate that theNorthAmerican oil and gas emissions of CH4, amajor greenhouse gas, grew from20 to 35 Tg yr −1 over the period 2008–2014, in associationwith the recent C2H6 rise.

Book ChapterDOI
TL;DR: Researchers have found that addition of conductive materials and/or electrically active cathodes to anaerobic digesters can stimulate the digestion process and increase methane content of biogas, which is a promising renewable energy source.
Abstract: Methanogens are a unique group of strictly anaerobic archaea that are more metabolically diverse than previously thought Traditionally, it was thought that methanogens could only generate methane by coupling the oxidation of products formed by fermentative bacteria with the reduction of CO2 However, it has recently been observed that many methanogens can also use electrons extruded from metal-respiring bacteria, biocathodes, or insoluble electron shuttles as energy sources Methanogens are found in both human-made and natural environments and are responsible for the production of ∼71% of the global atmospheric methane Their habitats range from the human digestive tract to hydrothermal vents Although biologically produced methane can negatively impact the environment if released into the atmosphere, when captured, it can serve as a potent fuel source The anaerobic digestion of wastes such as animal manure, human sewage, or food waste produces biogas which is composed of ∼60% methane Methane from biogas can be cleaned to yield purified methane (biomethane) that can be readily incorporated into natural gas pipelines making it a promising renewable energy source Conventional anaerobic digestion is limited by long retention times, low organics removal efficiencies, and low biogas production rates Therefore, many studies are being conducted to improve the anaerobic digestion process Researchers have found that addition of conductive materials and/or electrically active cathodes to anaerobic digesters can stimulate the digestion process and increase methane content of biogas It is hoped that optimization of anaerobic digesters will make biogas more readily accessible to the average person

Journal ArticleDOI
TL;DR: In this paper, in situ airborne measurements of methane (CH4) and ethane (C2H6) taken aboard a NOAA DHC-6 Twin Otter research aircraft in May 2014 over the Williston Basin in northwestern North Dakota, a region of rapidly growing oil and natural gas production.
Abstract: We present in situ airborne measurements of methane (CH4) and ethane (C2H6) taken aboard a NOAA DHC-6 Twin Otter research aircraft in May 2014 over the Williston Basin in northwestern North Dakota, a region of rapidly growing oil and natural gas production. The Williston Basin is best known for the Bakken shale formation, from which a significant increase in oil and gas extraction has occurred since 2009. We derive a CH4 emission rate from this region using airborne data by calculating the CH4 enhancement flux through the planetary boundary layer downwind of the region. We calculate CH4 emissions of (36 ± 13), (27 ± 13), (27 ± 12), (27 ± 12), and (25 ± 10) × 103 kg/h from five transects on 3 days in May 2014 downwind of the Bakken shale region of North Dakota. The average emission, (28 ± 5) × 103 kg/h, extrapolates to 0.25 ± 0.05 Tg/yr, which is significantly lower than a previous estimate of CH4 emissions from northwestern North Dakota and southeastern Saskatchewan using satellite remote sensing data. We attribute the majority of CH4 emissions in the region to oil and gas operations in the Bakken based on the similarity between atmospheric C2H6 to CH4 enhancement ratios and the composition of raw natural gas withdrawn from the region.

Posted ContentDOI
TL;DR: In this article, the authors used the GEOS-Chem chemical transport model tagged simulation that accounts for the contribution of each emission source and one sink in the total methane, simulated over the 2005-2012 time period and based on emissions inventories and transport.
Abstract: Changes of atmospheric methane (CH4) since 2005 have been evaluated using Fourier Transform Infrared (FTIR) solar observations performed at ten ground-based sites, all members of the Network for Detection of Atmospheric Composition 25 Change (NDACC). From this, we find an increase of atmospheric methane total columns that amounts to 0.31 ± 0.03 % year (2-sigma level of uncertainty) for the 2005-2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem Chemical Transport Model tagged simulation that accounts for the contribution of each emission source and one sink in the total methane, simulated over the 2005-2012 time period and based on emissions inventories and transport. After regridding according to NDACC vertical layering using a conservative 30 regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane of 0.35 ± 0.03 % year between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year, averaged over ten stations). Analysis of the GEOS-Chem tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the inter-annual variability of methane. 35 However, anthropogenic emissions such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained. 40 Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-699, 2016 Manuscript under review for journal Atmos. Chem. Phys. Published: 9 August 2016 c © Author(s) 2016. CC-BY 3.0 License.

Journal ArticleDOI
TL;DR: The conversion of rice paddies to inland aquaculture would benefit for reconciling greenhouse gas mitigation and agricultural income increase as far as global warming potentials and net ecosystem economic profits are of concomitant concern, and more field measurements are highly needed to gain an insight into national and global accounting of CH4 and N2O emissions.
Abstract: Aquaculture is an important source of atmospheric methane (CH4) and nitrous oxide (N2O), while few direct flux measurements are available for their regional and global source strength estimates. A parallel field experiment was performed to measure annual CH4 and N2O fluxes from rice paddies and rice paddy-converted inland crab–fish aquaculture wetlands in southeast China. Besides N2O fluxes dependent on water/sediment mineral N and CH4 fluxes related to water chemical oxygen demand, both CH4 and N2O fluxes from aquaculture were related to water/sediment temperature, sediment dissolved organic carbon, and water dissolved oxygen concentration. Annual CH4 and N2O fluxes from inland aquaculture averaged 0.37 mg m–2 h–1 and 48.1 μg m–2 h–1, yielding 32.57 kg ha–1 and 2.69 kg N2O–N ha–1, respectively. The conversion of rice paddies to aquaculture significantly reduced CH4 and N2O emissions by 48% and 56%, respectively. The emission factor for N2O was estimated to be 0.66% of total N input in the feed or 1.64 g ...

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TL;DR: There is strong evidence that methane emissions from fossil fuel sectors were approximately constant in the 1980s and 1990s but increased significantly between 2000 and 2009, and this finding challenges recent conclusions based on atmospheric ethane that fugitive fossil fuel emissions fell during much of this period.
Abstract: Observations of atmospheric methane (CH4) since the late 1970s and measurements of CH4 trapped in ice and snow reveal a meteoric rise in concentration during much of the twentieth century. Since 1750, levels of atmospheric CH4 have more than doubled to current globally averaged concentration near 1,800 ppb. During the late 1980s and 1990s, the CH4 growth rate slowed substantially and was near or at zero between 1999 and 2006. There is no scientific consensus on the drivers of this slowdown. Here, we report measurements of the stable isotopic composition of atmospheric CH4 ((13)C/(12)C and D/H) from a rare air archive dating from 1977 to 1998. Together with more modern records of isotopic atmospheric CH4, we performed a time-dependent retrieval of methane fluxes spanning 25 y (1984-2009) using a 3D chemical transport model. This inversion results in a 24 [18, 27] Tg y(-1) CH4 increase in fugitive fossil fuel emissions since 1984 with most of this growth occurring after year 2000. This result is consistent with some bottom-up emissions inventories but not with recent estimates based on atmospheric ethane. In fact, when forced with decreasing emissions from fossil fuel sources our inversion estimates unreasonably high emissions in other sources. Further, the inversion estimates a decrease in biomass-burning emissions that could explain falling ethane abundance. A range of sensitivity tests suggests that these results are robust.

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TL;DR: In this paper, a 3-D global chemical transport model was used to investigate CH4 growth variations, and the model showed 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.
Abstract: . 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.

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TL;DR: In this article, a comparison of high-resolution simulations of atmospheric methane mole fractions to continuous methane observations during the whole year 2012 confirms the high variability and heterogeneity of the methane releases from the East Siberian Arctic Shelf.
Abstract: . Subsea permafrost and hydrates in the East Siberian Arctic Shelf (ESAS) constitute a substantial carbon pool, and a potentially large source of methane to the atmosphere. Previous studies based on interpolated oceanographic campaigns estimated atmospheric emissions from this area at 8–17 TgCH4 yr−1. Here, we propose insights based on atmospheric observations to evaluate these estimates. The comparison of high-resolution simulations of atmospheric methane mole fractions to continuous methane observations during the whole year 2012 confirms the high variability and heterogeneity of the methane releases from ESAS. A reference scenario with ESAS emissions of 8 TgCH4 yr−1, in the lower part of previously estimated emissions, is found to largely overestimate atmospheric observations in winter, likely related to overestimated methane leakage through sea ice. In contrast, in summer, simulations are more consistent with observations. Based on a comprehensive statistical analysis of the observations and of the simulations, annual methane emissions from ESAS are estimated to range from 0.0 to 4.5 TgCH4 yr−1. Isotopic observations suggest a biogenic origin (either terrestrial or marine) of the methane in air masses originating from ESAS during late summer 2008 and 2009.

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TL;DR: In this article, the authors investigate the atmospheric CH4 evolution over the period 1970-2012 with the Oslo CTM3 global chemical transport model (CTM) in a bottom-up approach.
Abstract: . Observations at surface sites show an increase in global mean surface methane (CH4) of about 180 parts per billion (ppb) (above 10 %) over the period 1984–2012. Over this period there are large fluctuations in the annual growth rate. In this work, we investigate the atmospheric CH4 evolution over the period 1970–2012 with the Oslo CTM3 global chemical transport model (CTM) in a bottom-up approach. We thoroughly assess data from surface measurement sites in international networks and select a subset suited for comparisons with the output from the CTM. We compare model results and observations to understand causes for both long-term trends and short-term variations. Employing Oslo CTM3 we are able to reproduce the seasonal and year-to-year variations and shifts between years with consecutive growth and stagnation, both at global and regional scales. The overall CH4 trend over the period is reproduced, but for some periods the model fails to reproduce the strength of the growth. The model overestimates the observed growth after 2006 in all regions. This seems to be explained by an overly strong increase in anthropogenic emissions in Asia, having global impact. Our findings confirm other studies questioning the timing or strength of the emission changes in Asia in the EDGAR v4.2 emission inventory over recent decades. The evolution of CH4 is not only controlled by changes in sources, but also by changes in the chemical loss in the atmosphere and soil uptake. The atmospheric CH4 lifetime is an indicator of the CH4 loss. In our simulations, the atmospheric CH4 lifetime decreases by more than 8 % from 1970 to 2012, a significant reduction of the residence time of this important greenhouse gas. Changes in CO and NOx emissions, specific humidity, and ozone column drive most of this, and we provide simple prognostic equations for the relations between those and the CH4 lifetime. The reduced lifetime results in substantial growth in the chemical CH4 loss (relative to its burden) and dampens the CH4 growth.

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TL;DR: In this article, the authors apply measurements of multiply-substituted isotopologues, or clumped isotopes, of methane as a new tool to identify the origins of ebullitive fluxes in Alaska, Sweden and the Arctic Ocean.

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TL;DR: In this paper, the authors used a simple and fast data-driven method to estimate annual methane emissions and corresponding 1σ uncertainties directly from maps of annually averaged satellite XCH4.
Abstract: . Methane is an important atmospheric greenhouse gas and an adequate understanding of its emission sources is needed for climate change assessments, predictions, and the development and verification of emission mitigation strategies. Satellite retrievals of near-surface-sensitive column-averaged dry-air mole fractions of atmospheric methane, i.e. XCH4, can be used to quantify methane emissions. Maps of time-averaged satellite-derived XCH4 show regionally elevated methane over several methane source regions. In order to obtain methane emissions of these source regions we use a simple and fast data-driven method to estimate annual methane emissions and corresponding 1σ uncertainties directly from maps of annually averaged satellite XCH4. From theoretical considerations we expect that our method tends to underestimate emissions. When applying our method to high-resolution atmospheric methane simulations, we typically find agreement within the uncertainty range of our method (often 100 %) but also find that our method tends to underestimate emissions by typically about 40 %. To what extent these findings are model dependent needs to be assessed. We apply our method to an ensemble of satellite XCH4 data products consisting of two products from SCIAMACHY/ENVISAT and two products from TANSO-FTS/GOSAT covering the time period 2003–2014. We obtain annual emissions of four source areas: Four Corners in the south-western USA, the southern part of Central Valley, California, Azerbaijan, and Turkmenistan. We find that our estimated emissions are in good agreement with independently derived estimates for Four Corners and Azerbaijan. For the Central Valley and Turkmenistan our estimated annual emissions are higher compared to the EDGAR v4.2 anthropogenic emission inventory. For Turkmenistan we find on average about 50 % higher emissions with our annual emission uncertainty estimates overlapping with the EDGAR emissions. For the region around Bakersfield in the Central Valley we find a factor of 5–8 higher emissions compared to EDGAR, albeit with large uncertainty. Major methane emission sources in this region are oil/gas and livestock. Our findings corroborate recently published studies based on aircraft and satellite measurements and new bottom-up estimates reporting significantly underestimated methane emissions of oil/gas and/or livestock in this area in EDGAR.

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TL;DR: This review highlights and discusses the interplay between ammonia and methane oxidizing bacteria, the potential interactions of microbial communities with microbially-enriched organic amendments and the possible role of these biofertilizers in augmenting the methane sink potential of soils.

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TL;DR: In this paper, the present and future contribution to atmospheric CH4 from lakes, wetlands, fluvial systems, and, potentially, coastal waters is quantified for the first time.
Abstract: Quantification of the present and future contribution to atmospheric methane (CH4) from lakes, wetlands, fluvial systems, and, potentially, coastal waters remains an important unfinished task for b ...

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TL;DR: In this paper, the authors show that even the observed short-term temperature sensitivity from the Arctic will have little impact on the global atmospheric CH4 budget in the long term if future trajectories evolve with the same temperature sensitivity.
Abstract: Continuous measurements of atmospheric methane (CH4) mole fractions measured by NOAA's Global Greenhouse Gas Reference Network in Barrow, AK (BRW), show strong enhancements above background values when winds come from the land sector from July to December from 1986 to 2015, indicating that emissions from arctic tundra continue through autumn and into early winter. Twenty-nine years of measurements show little change in seasonal mean land sector CH4 enhancements, despite an increase in annual mean temperatures of 1.2 ± 0.8°C/decade (2σ). The record does reveal small increases in CH4 enhancements in November and December after 2010 due to increased late-season emissions. The lack of significant long-term trends suggests that more complex biogeochemical processes are counteracting the observed short-term (monthly) temperature sensitivity of 5.0 ± 3.6 ppb CH4/°C. Our results suggest that even the observed short-term temperature sensitivity from the Arctic will have little impact on the global atmospheric CH4 budget in the long term if future trajectories evolve with the same temperature sensitivity.