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Showing papers on "Atmospheric methane published in 2017"


Journal ArticleDOI
TL;DR: It is concluded that the current surface observing system does not allow unambiguous attribution of the decadal trends in methane without robust constraints on OH variability, which currently rely purely on methyl chloroform data and its uncertain emissions estimates.
Abstract: Methane is the second strongest anthropogenic greenhouse gas and its atmospheric burden has more than doubled since 1850. Methane concentrations stabilized in the early 2000s and began increasing again in 2007. Neither the stabilization nor the recent growth are well understood, as evidenced by multiple competing hypotheses in recent literature. Here we use a multispecies two-box model inversion to jointly constrain 36 y of methane sources and sinks, using ground-based measurements of methane, methyl chloroform, and the C13/C12 ratio in atmospheric methane (δ13CH4) from 1983 through 2015. We find that the problem, as currently formulated, is underdetermined and solutions obtained in previous work are strongly dependent on prior assumptions. Based on our analysis, the mathematically most likely explanation for the renewed growth in atmospheric methane, counterintuitively, involves a 25-Tg/y decrease in methane emissions from 2003 to 2016 that is offset by a 7% decrease in global mean hydroxyl (OH) concentrations, the primary sink for atmospheric methane, over the same period. However, we are still able to fit the observations if we assume that OH concentrations are time invariant (as much of the previous work has assumed) and we then find solutions that are largely consistent with other proposed hypotheses for the renewed growth of atmospheric methane since 2007. We conclude that the current surface observing system does not allow unambiguous attribution of the decadal trends in methane without robust constraints on OH variability, which currently rely purely on methyl chloroform data and its uncertain emissions estimates.

216 citations


Journal ArticleDOI
14 Dec 2017-Nature
TL;DR: Close agreement is found between the ‘top-down’ and combined ‘bottom-up’ estimates of large CH4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH4 budget.
Abstract: Wetlands are the largest global source of atmospheric methane (CH4), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH4 in the tropics, consistently underestimate the atmospheric burden of CH4 determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH4 emissions. Here we report CH4 fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH4 emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δ13C) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH4 a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a 'top-down' regional estimate of CH4 emissions of 42.7 ± 5.6 teragrams of CH4 a year for the Amazon basin, based on regular vertical lower-troposphere CH4 profiles covering the period 2010-2013. We find close agreement between our 'top-down' and combined 'bottom-up' estimates, indicating that large CH4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH4 budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH4 emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH4 source when trees are combined with other emission sources.

188 citations


Journal ArticleDOI
TL;DR: It is shown that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH4 per year from the 2001–2007 to the 2008–2014 time periods using satellite measurements of CO and CH4, nearly twice the decrease expected from prior estimates.
Abstract: Several viable but conflicting explanations have been proposed to explain the recent ~8 p.p.b. per year increase in atmospheric methane after 2006, equivalent to net emissions increase of ~25 Tg CH4 per year. A concurrent increase in atmospheric ethane implicates a fossil source; a concurrent decrease in the heavy isotope content of methane points toward a biogenic source, while other studies propose a decrease in the chemical sink (OH). Here we show that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH4 per year from the 2001–2007 to the 2008–2014 time periods using satellite measurements of CO and CH4, nearly twice the decrease expected from prior estimates. After updating both the total and isotopic budgets for atmospheric methane with these revised biomass burning emissions (and assuming no change to the chemical sink), we find that fossil fuels contribute between 12–19 Tg CH4 per year to the recent atmospheric methane increase, thus reconciling the isotopic- and ethane-based results. The drivers of the increase in atmospheric methane since 2006 remain unclear. Here, the authors use satellite and in situ measurements of CO and CH4 to show that fossil fuels and biogenic sources contribute 12–19 Tg CH4per year and 12–16 Tg CH4per year respectively to the recent atmospheric methane increase.

175 citations


Journal ArticleDOI
TL;DR: In this article, a global wetland CH4 emission model ensemble for use in atmospheric chemical transport models (WetCHARTs version 1.0) is presented, which is based on satellite-derived surface water extent and precipitation reanalyses.
Abstract: . Wetland emissions remain one of the principal sources of uncertainty in the global atmospheric methane (CH4) budget, largely due to poorly constrained process controls on CH4 production in waterlogged soils. Process-based estimates of global wetland CH4 emissions and their associated uncertainties can provide crucial prior information for model-based top-down CH4 emission estimates. Here we construct a global wetland CH4 emission model ensemble for use in atmospheric chemical transport models (WetCHARTs version 1.0). Our 0.5° × 0.5° resolution model ensemble is based on satellite-derived surface water extent and precipitation reanalyses, nine heterotrophic respiration simulations (eight carbon cycle models and a data-constrained terrestrial carbon cycle analysis) and three temperature dependence parameterizations for the period 2009–2010; an extended ensemble subset based solely on precipitation and the data-constrained terrestrial carbon cycle analysis is derived for the period 2001–2015. We incorporate the mean of the full and extended model ensembles into GEOS-Chem and compare the model against surface measurements of atmospheric CH4; the model performance (site-level and zonal mean anomaly residuals) compares favourably against published wetland CH4 emissions scenarios. We find that uncertainties in carbon decomposition rates and the wetland extent together account for more than 80 % of the dominant uncertainty in the timing, magnitude and seasonal variability in wetland CH4 emissions, although uncertainty in the temperature CH4 : C dependence is a significant contributor to seasonal variations in mid-latitude wetland CH4 emissions. The combination of satellite, carbon cycle models and temperature dependence parameterizations provides a physically informed structural a priori uncertainty that is critical for top-down estimates of wetland CH4 fluxes. Specifically, our ensemble can provide enhanced information on the prior CH4 emission uncertainty and the error covariance structure, as well as a means for using posterior flux estimates and their uncertainties to quantitatively constrain the biogeochemical process controls of global wetland CH4 emissions.

152 citations


Journal ArticleDOI
TL;DR: In this article, the authors provided an updated estimate of CH4 emissions from wetlands, the largest natural global CH4 source, for 2000-2012 using an ensemble of biogeochemical models constrained with remote sensing surface inundation and inventory-based wetland area data.
Abstract: Increasing atmospheric methane (CH4) concentrations have contributed to approximately 20% of anthropogenic climate change. Despite the importance of CH4 as a greenhouse gas, its atmospheric growth rate and dynamics over the past two decades, which include a stabilization period (1999–2006), followed by renewed growth starting in 2007, remain poorly understood. We provide an updated estimate of CH4 emissions from wetlands, the largest natural global CH4 source, for 2000–2012 using an ensemble of biogeochemical models constrained with remote sensing surface inundation and inventory-based wetland area data. Between 2000–2012, boreal wetland CH4 emissions increased by 1.2 Tg yr−1 (−0.2–3.5 Tg yr−1), tropical emissions decreased by 0.9 Tg yr−1 (−3.2−1.1 Tg yr−1), yet globally, emissions remained unchanged at 184 ± 22 Tg yr−1. Changing air temperature was responsible for increasing high-latitude emissions whereas declines in low-latitude wetland area decreased tropical emissions; both dynamics are consistent with features of predicted centennial-scale climate change impacts on wetland CH4 emissions. Despite uncertainties in wetland area mapping, our study shows that global wetland CH4 emissions have not contributed significantly to the period of renewed atmospheric CH4 growth, and is consistent with findings from studies that indicate some combination of increasing fossil fuel and agriculture-related CH4 emissions, and a decrease in the atmospheric oxidative sink.

140 citations


Journal ArticleDOI
TL;DR: In this paper, the authors presented a comprehensive, globally representative end-member database of the δ13C and δ2H of CH4 from fossil fuel (conventional natural gas, shale gas, and coal), modern microbial (wetlands, rice paddies, ruminants, termites, and landfills and/or waste) and biomass burning sources.
Abstract: . The concentration of atmospheric methane (CH4) has more than doubled over the industrial era. To help constrain global and regional CH4 budgets, inverse (top-down) models incorporate data on the concentration and stable carbon (δ13C) and hydrogen (δ2H) isotopic ratios of atmospheric CH4. These models depend on accurate δ13C and δ2H end-member source signatures for each of the main emissions categories. Compared with meticulous measurement and calibration of isotopic CH4 in the atmosphere, there has been relatively less effort to characterize globally representative isotopic source signatures, particularly for fossil fuel sources. Most global CH4 budget models have so far relied on outdated source signature values derived from globally nonrepresentative data. To correct this deficiency, we present a comprehensive, globally representative end-member database of the δ13C and δ2H of CH4 from fossil fuel (conventional natural gas, shale gas, and coal), modern microbial (wetlands, rice paddies, ruminants, termites, and landfills and/or waste) and biomass burning sources. Gas molecular compositional data for fossil fuel categories are also included with the database. The database comprises 10 706 samples (8734 fossil fuel, 1972 non-fossil) from 190 published references. Mean (unweighted) δ13C signatures for fossil fuel CH4 are significantly lighter than values commonly used in CH4 budget models, thus highlighting potential underestimation of fossil fuel CH4 emissions in previous CH4 budget models. This living database will be updated every 2–3 years to provide the atmospheric modeling community with the most complete CH4 source signature data possible. Database digital object identifier (DOI): https://doi.org/10.15138/G3201T .

123 citations


Journal ArticleDOI
TL;DR: It is suggested that microbial reduction of NOM may largely contribute to the suppression of methane emissions from tropical wetlands, a novel avenue within the carbon cycle in which slowly decaying NOM in organotrophic environments fuels AOM by serving as a terminal electron acceptor.
Abstract: Wetlands constitute the main natural source of methane on Earth due to their high content of natural organic matter (NOM), but key drivers, such as electron acceptors, supporting methanotrophic activities in these habitats are poorly understood. We performed anoxic incubations using freshly collected sediment, along with water samples harvested from a tropical wetland, amended with 13C-methane (0.67 atm) to test the capacity of its microbial community to perform anaerobic oxidation of methane (AOM) linked to the reduction of the humic fraction of its NOM. Collected evidence demonstrates that electron-accepting functional groups (e.g., quinones) present in NOM fueled AOM by serving as a terminal electron acceptor. Indeed, while sulfate reduction was the predominant process, accounting for up to 42.5% of the AOM activities, the microbial reduction of NOM concomitantly occurred. Furthermore, enrichment of wetland sediment with external NOM provided a complementary electron-accepting capacity, of which reduction accounted for ∼100 nmol 13CH4 oxidized · cm-3 · day-1 Spectroscopic evidence showed that quinone moieties were heterogeneously distributed in the wetland sediment, and their reduction occurred during the course of AOM. Moreover, an enrichment derived from wetland sediments performing AOM linked to NOM reduction stoichiometrically oxidized methane coupled to the reduction of the humic analogue anthraquinone-2,6-disulfonate. Microbial populations potentially involved in AOM coupled to microbial reduction of NOM were dominated by divergent biota from putative AOM-associated archaea. We estimate that this microbial process potentially contributes to the suppression of up to 114 teragrams (Tg) of CH4 · year-1 in coastal wetlands and more than 1,300 Tg · year-1, considering the global wetland area.IMPORTANCE The identification of key processes governing methane emissions from natural systems is of major importance considering the global warming effects triggered by this greenhouse gas. Anaerobic oxidation of methane (AOM) coupled to the microbial reduction of distinct electron acceptors plays a pivotal role in mitigating methane emissions from ecosystems. Given their high organic content, wetlands constitute the largest natural source of atmospheric methane. Nevertheless, processes controlling methane emissions in these environments are poorly understood. Here, we provide tracer analysis with 13CH4 and spectroscopic evidence revealing that AOM linked to the microbial reduction of redox functional groups in natural organic matter (NOM) prevails in a tropical wetland. We suggest that microbial reduction of NOM may largely contribute to the suppression of methane emissions from tropical wetlands. This is a novel avenue within the carbon cycle in which slowly decaying NOM (e.g., humic fraction) in organotrophic environments fuels AOM by serving as a terminal electron acceptor.

107 citations


Journal ArticleDOI
TL;DR: In this paper, the Global Carbon Project (GCP) synthesis of the decadal CH4 budget over 2000-2012 (Saunois et al., 2016) was analyzed with a focus on quasi-decadal and inter-annual variability in CH4 emissions.
Abstract: Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000-2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32]Tg CH4yr-1 higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

100 citations


Journal ArticleDOI
TL;DR: In this article, the authors used measurements of methane concentrations and stable isotope compositions along with genomic analyses to assess the sources and cycling of methane in Subglacial Lake Whillans (SLW) in West Antarctica.
Abstract: Aquatic habitats beneath ice masses contain active microbial ecosystems capable of cycling important greenhouse gases, such as methane (CH4). A large methane reservoir is thought to exist beneath the West Antarctic Ice Sheet, but its quantity, source and ultimate fate are poorly understood. For instance, O2 supplied by basal melting should result in conditions favourable for aerobic methane oxidation. Here we use measurements of methane concentrations and stable isotope compositions along with genomic analyses to assess the sources and cycling of methane in Subglacial Lake Whillans (SLW) in West Antarctica. We show that sub-ice-sheet methane is produced through the biological reduction of CO2 using H2. This methane pool is subsequently consumed by aerobic, bacterial methane oxidation at the SLW sediment–water interface. Bacterial oxidation consumes >99% of the methane and represents a significant methane sink, and source of biomass carbon and metabolic energy to the surficial SLW sediments. We conclude that aerobic methanotrophy may mitigate the release of methane to the atmosphere upon subglacial water drainage to ice sheet margins and during periods of deglaciation. Subglacial lakes contain active microbial ecosystems capable of cycling methane. In a subglacial lake in West Antarctica, methane that is produced is subsequently consumed, limiting the potential for methane emissions during lake drainage.

82 citations


Journal ArticleDOI
TL;DR: Overall, wet-gas basins had higher TNMA emissions than the dry-gas FV at all ranges of production per well pad, suggesting that consolidation of operations onto single pads may reduce normalized emissions.
Abstract: Atmospheric methane emissions from active natural gas production sites in normal operation were quantified using an inverse Gaussian method (EPA’s OTM 33a) in four major U.S. basins/plays: Upper Green River (UGR, Wyoming), Denver-Julesburg (DJ, Colorado), Uintah (Utah), and Fayetteville (FV, Arkansas). In DJ, Uintah, and FV, 72–83% of total measured emissions were from 20% of the well pads, while in UGR the highest 20% of emitting well pads only contributed 54% of total emissions. The total mass of methane emitted as a percent of gross methane produced, termed throughput-normalized methane average (TNMA) and determined by bootstrapping measurements from each basin, varied widely between basins and was (95% CI): 0.09% (0.05–0.15%) in FV, 0.18% (0.12–0.29%) in UGR, 2.1% (1.1–3.9%) in DJ, and 2.8% (1.0–8.6%) in Uintah. Overall, wet-gas basins (UGR, DJ, Uintah) had higher TNMA emissions than the dry-gas FV at all ranges of production per well pad. Among wet basins, TNMA emissions had a strong negative correla...

81 citations


Journal ArticleDOI
TL;DR: The MERLIN objectives are presented, the methodology and the main characteristics of the payload and of the platform are described, and a first assessment of the error budget and its translation into expected uncertainty reduction of methane surface emissions is proposed.
Abstract: The MEthane Remote sensing Lidar missioN (MERLIN) aims at demonstrating the spaceborne active measurement of atmospheric methane, a potent greenhouse gas, based on an Integrated Path Differential Absorption (IPDA) nadir-viewing LIght Detecting and Ranging (Lidar) instrument. MERLIN is a joint French and German space mission, with a launch currently scheduled for the timeframe 2021/22. The German Space Agency (DLR) is responsible for the payload, while the platform (MYRIADE Evolutions product line) is developed by the French Space Agency (CNES). The main scientific objective of MERLIN is the delivery of weighted atmospheric columns of methane dry-air mole fractions for all latitudes throughout the year with systematic errors small enough (<3.7 ppb) to significantly improve our knowledge of methane sources from global to regional scales, with emphasis on poorly accessible regions in the tropics and at high latitudes. This paper presents the MERLIN objectives, describes the methodology and the main characteristics of the payload and of the platform, and proposes a first assessment of the error budget and its translation into expected uncertainty reduction of methane surface emissions.

Journal ArticleDOI
23 Aug 2017-Nature
TL;DR: To the extent that the characteristics of the most recent deglaciation and the Younger Dryas–Preboreal warming are comparable to those of the current anthropogenic warming, the measurements suggest that large future atmospheric releases of methane from old carbon sources are unlikely to occur.
Abstract: Methane (CH$_4$) is a powerful greenhouse gas and plays a key part in global atmospheric chemistry. Natural geological emissions (fossil methane vented naturally from marine and terrestrial seeps and mud volcanoes) are thought to contribute around 52 teragrams of methane per year to the global methane source, about 10 per cent of the total, but both bottom-up methods (measuring emissions)1 and top-down approaches (measuring atmospheric mole fractions and isotopes)2 for constraining these geological emissions have been associated with large uncertainties. Here we use ice core measurements to quantify the absolute amount of radiocarbon-containing methane ($^{14}$CH$_4$) in the past atmosphere and show that geological methane emissions were no higher than 15.4 teragrams per year (95 per cent confidence), averaged over the abrupt warming event that occurred between the Younger Dryas and Preboreal intervals, approximately 11,600 years ago. Assuming that past geological methane emissions were no lower than today 3,4, our results indicate that current estimates of today’s natural geological methane emissions (about 52 teragrams per year)1,2 are too high and, by extension, that current estimates of anthropogenic fossil methane emissions 2 are too low. Our results also improve on and confirm earlier findings5,6,7 that the rapid increase of about 50 per cent in mole fraction of atmospheric methane at the Younger Dryas–Preboreal event was driven by contemporaneous methane from sources such as wetlands; our findings constrain the contribution from old carbon reservoirs (marine methane hydrates8, permafrost9 and methane trapped under ice10) to 19 per cent or less (95 per cent confidence). To the extent that the characteristics of the most recent deglaciation and the Younger Dryas–Preboreal warming are comparable to those of the current anthropogenic warming, our measurements suggest that large future atmospheric releases of methane from old carbon sources are unlikely to occur.

Journal ArticleDOI
TL;DR: The Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed.
Abstract: Emerging evidence suggests that atmospheric oxygen may have varied before rising irreversibly ∼2.4 billion years ago, during the Great Oxidation Event (GOE). Significantly, however, pre-GOE atmospheric aberrations toward more reducing conditions-featuring a methane-derived organic-haze-have recently been suggested, yet their occurrence, causes, and significance remain underexplored. To examine the role of haze formation in Earth's history, we targeted an episode of inferred haze development. Our redox-controlled (Fe-speciation) carbon- and sulfur-isotope record reveals sustained systematic stratigraphic covariance, precluding nonatmospheric explanations. Photochemical models corroborate this inference, showing Δ36S/Δ33S ratios are sensitive to the presence of haze. Exploiting existing age constraints, we estimate that organic haze developed rapidly, stabilizing within ∼0.3 ± 0.1 million years (Myr), and persisted for upward of ∼1.4 ± 0.4 Myr. Given these temporal constraints, and the elevated atmospheric CO2 concentrations in the Archean, the sustained methane fluxes necessary for haze formation can only be reconciled with a biological source. Correlative δ13COrg and total organic carbon measurements support the interpretation that atmospheric haze was a transient response of the biosphere to increased nutrient availability, with methane fluxes controlled by the relative availability of organic carbon and sulfate. Elevated atmospheric methane concentrations during haze episodes would have expedited planetary hydrogen loss, with a single episode of haze development providing up to 2.6-18 × 1018 moles of O2 equivalents to the Earth system. Our findings suggest the Neoarchean likely represented a unique state of the Earth system where haze development played a pivotal role in planetary oxidation, hastening the contingent biological innovations that followed.

Journal ArticleDOI
TL;DR: This article reported that CH4 emissions from the stems of dominant tree species in a temperate upland forest, measured using both the traditional static-chamber method and a new high-frequency, automated system.
Abstract: Summary Global budgets ascribe 4–10% of atmospheric methane (CH4) sinks to upland soils and have assumed until recently that soils are the sole surface for CH4 exchange in upland forests. Here we report that CH4 is emitted from the stems of dominant tree species in a temperate upland forest, measured using both the traditional static-chamber method and a new high-frequency, automated system. Tree emissions averaged across 68 observations on 17 trees from May to September were 1.59 ± 0.88 μmol CH4 m−2 stem h−1 (mean ± 95% confidence interval), while soils adjacent to the trees consumed atmospheric CH4 at a rate of −4.52 ± 0.64 μmol CH4 m−2 soil h−1 (P < 0.0001). High-frequency measurements revealed diurnal patterns in the rate of tree-stem CH4 emissions. A simple scaling exercise suggested that tree emissions offset 1–6% of the growing season soil CH4 sink and may have briefly changed the forest to a net CH4 source.

Journal ArticleDOI
TL;DR: The results indicate that under natural conditions where both hydrogen and methane might be limiting strain SolV may operate primarily as a methanotrophic ‘Knallgas’ bacterium, and argue for a revision of the role of hydrogen in methanOTrophic ecosystems.
Abstract: Methanotrophs play a key role in balancing the atmospheric methane concentration. Recently, the microbial methanotrophic diversity was extended by the discovery of thermoacidophilic methanotrophs belonging to the Verrucomicrobia phylum in geothermal areas. Here we show that a representative of this new group, Methylacidiphilum fumariolicum SolV, is able to grow as a real ‘Knallgas’ bacterium on hydrogen/carbon dioxide, without addition of methane. The full genome of strain SolV revealed the presence of two hydrogen uptake hydrogenases genes, encoding an oxygen-sensitive (hup-type) and an oxygen-insensitive enzyme (hhy-type). The hhy-type hydrogenase was constitutively expressed and active and supported growth on hydrogen alone up to a growth rate of 0.03 h−1, at O2 concentrations below 1.5%. The oxygen-sensitive hup-type hydrogenase was expressed when oxygen was reduced to below 0.2%. This resulted in an increase of the growth rate to a maximum of 0.047 h−1, that is 60% of the rate on methane. The results indicate that under natural conditions where both hydrogen and methane might be limiting strain SolV may operate primarily as a methanotrophic ‘Knallgas’ bacterium. These findings argue for a revision of the role of hydrogen in methanotrophic ecosystems, especially in soil and related to consumption of atmospheric methane.

Journal ArticleDOI
TL;DR: Ganesan et al. as mentioned in this paper derived India's methane emissions for the period 2010-2015 using a combination of satellite, surface and aircraft data and applied a high-resolution atmospheric transport model to simulate data from these platforms to infer fluxes at sub-national scales and quantify changes in rice emissions.
Abstract: Changes in tropical wetland, ruminant or rice emissions are thought to have played a role in recent variations in atmospheric methane (CH4) 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 CH4 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 CH4 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.

Journal ArticleDOI
TL;DR: Dual stable isotopic methane records from four Antarctic ice cores provide improved constraints on past changes in natural methane sources and show that tropical wetlands and seasonally inundated floodplains are most likely the controlling sources of atmospheric methane variations for the current and two older interglacials and their preceding glacial maxima.
Abstract: Atmospheric methane (CH4) records reconstructed from polar ice cores represent an integrated view on processes predominantly taking place in the terrestrial biogeosphere. Here, we present dual stable isotopic methane records [δ13CH4 and δD(CH4)] from four Antarctic ice cores, which provide improved constraints on past changes in natural methane sources. Our isotope data show that tropical wetlands and seasonally inundated floodplains are most likely the controlling sources of atmospheric methane variations for the current and two older interglacials and their preceding glacial maxima. The changes in these sources are steered by variations in temperature, precipitation, and the water table as modulated by insolation, (local) sea level, and monsoon intensity. Based on our δD(CH4) constraint, it seems that geologic emissions of methane may play a steady but only minor role in atmospheric CH4 changes and that the glacial budget is not dominated by these sources. Superimposed on the glacial/interglacial variations is a marked difference in both isotope records, with systematically higher values during the last 25,000 y compared with older time periods. This shift cannot be explained by climatic changes. Rather, our isotopic methane budget points to a marked increase in fire activity, possibly caused by biome changes and accumulation of fuel related to the late Pleistocene megafauna extinction, which took place in the course of the last glacial.

Journal ArticleDOI
TL;DR: This article showed that outgassed methane can build up to atmospheric levels sufficient for lake-forming climates, if methane clathrate initially occupies more than 4% of the total volume in which it is thermodynamically stable.
Abstract: Lakes existed on Mars later than 3.6 billion years ago, according to sedimentary evidence for deltaic deposition. The observed fluviolacustrine deposits suggest that individual lake-forming climates persisted for at least several thousand years (assuming dilute flow). But the lake watersheds’ little-weathered soils indicate a largely dry climate history, with intermittent runoff events. Here we show that these observational constraints, although inconsistent with many previously proposed triggers for lake-forming climates, are consistent with a methane burst scenario. In this scenario, chaotic transitions in mean obliquity drive latitudinal shifts in temperature and ice loading that destabilize methane clathrate. Using numerical simulations, we find that outgassed methane can build up to atmospheric levels sufficient for lake-forming climates, if methane clathrate initially occupies more than 4% of the total volume in which it is thermodynamically stable. Such occupancy fractions are consistent with methane production by water–rock reactions due to hydrothermal circulation on early Mars. We further estimate that photochemical destruction of atmospheric methane curtails the duration of individual lake-forming climates to less than a million years, consistent with observations. We conclude that methane bursts represent a potential pathway for intermittent excursions to a warm, wet climate state on early Mars. Bursts of methane stored in the Martian subsurface may explain intermittent warm climates on ancient Mars, according to numerical simulations. Sedimentary evidence for palaeolakes requires infrequent, yet sustained, lake-forming climates.

Journal ArticleDOI
TL;DR: In this article, a bottom-up approach was used to quantify and attribute methane and ethane emissions from global oil and gas production from 1980 to 2012, using country-specific information on associated gas flows from published sources.
Abstract: Existing bottom-up emission inventories of methane from global oil and gas systems do not satisfactorily explain year-on-year variation in atmospheric methane estimated by top-down models. Using a novel bottom-up approach this study quantifies and attributes methane and ethane emissions from global oil and gas production from 1980 to 2012. Country-specific information on associated gas flows from published sources are combined with inter-annual variations in observed flaring of associated gas from satellite images from 1994 to 2010, to arrive at country-specific annual estimates of methane and ethane emissions from flows of associated gas. Results confirm trends from top-down models and indicate considerably higher methane and ethane emissions from oil production than previously shown in bottom-up inventories for this time period.

Journal ArticleDOI
TL;DR: High precision stable isotope analysis of atmospheric methane can be used to give a better understanding of urban sources and their partition in a source mix and suggests that a revision of the source distribution given by the emission inventories is needed.
Abstract: A thorough understanding of methane sources is necessary to accomplish methane reduction targets. Urban environments, where a large variety of methane sources coexist, are one of the most complex areas to investigate. Methane sources are characterised by specific δ13C-CH4 signatures, so high precision stable isotope analysis of atmospheric methane can be used to give a better understanding of urban sources and their partition in a source mix. Diurnal measurements of methane and carbon dioxide mole fraction, and isotopic values at King’s College London, enabled assessment of the isotopic signal of the source mix in central London. Surveys with a mobile measurement system in the London region were also carried out for detection of methane plumes at near ground level, in order to evaluate the spatial allocation of sources suggested by the inventories. The measured isotopic signal in central London (−45.7 ±0.5‰) was more than 2‰ higher than the isotopic value calculated using emission inventories and updated δ13C-CH4 signatures. Besides, during the mobile surveys, many gas leaks were identified that are not included in the inventories. This suggests that a revision of the source distribution given by the emission inventories is needed.

Journal ArticleDOI
TL;DR: In this article, the performance of an off-the-shelf, low-cost, metal oxide based methane (CH4) gas sensor was investigated, and a sensor assembly was designed that powered the gas sensor and its resistive heater, provided ancillary temperature (T) and relative humidity (rH) measurements, and controlled sensor read-out and data storage.
Abstract: In order to expand current atmospheric methane monitoring capabilities, we investigated the performance of an off-the-shelf, low-cost, metal oxide based methane (CH4) gas sensor. A sensor assembly was designed that powered the gas sensor and its resistive heater, provided ancillary temperature (T) and relative humidity (rH) measurements, and controlled sensor read-out and data storage. After calibrating the gas sensor with respect to methane concentration ([CH4]), T, and rH, we were able to estimate the [CH4] of lab air over a period of 31 days for a large range of T and rH conditions with a systematic error of −1.0 ppm and a variable error within ±1.7 ppm. The sensor showed no significant drift in [CH4] estimate. We show that sensor accuracy can likely be improved by optimizing the voltage regulator that powers the gas sensor’s heater, and by measuring and compensating for the difference in partial oxygen pressure of the air that was sampled during calibration and validation experiments. Such improvements are expected to allow the use of the sensor assembly for fence-line methane monitoring, for example near fossil fuel extraction sites. In its current form, the sensor assembly is suitable for detecting fugitive methane from leak-prone equipment.

Journal ArticleDOI
TL;DR: In this paper, a process-based model was developed to simulate and quantify the uptake of atmospheric CH4 by soils at the global scale, and the authors showed that the improved structural and parametric representation of key drivers of soil methanotrophy in MeMo results in a better fit to observational data.
Abstract: . Soil bacteria known as methanotrophs are the sole biological sink for atmospheric methane (CH 4) , a potent greenhouse gas that is responsible for ∼ 20 % of the human-driven increase in radiative forcing since pre-industrial times. Soil methanotrophy is controlled by a plethora of factors, including temperature, soil texture, moisture and nitrogen content, resulting in spatially and temporally heterogeneous rates of soil methanotrophy. As a consequence, the exact magnitude of the global soil sink, as well as its temporal and spatial variability, remains poorly constrained. We developed a process-based model (Methanotrophy Model; MeMo v1.0) to simulate and quantify the uptake of atmospheric CH4 by soils at the global scale. MeMo builds on previous models by Ridgwell et al. (1999) and Curry (2007) by introducing several advances, including (1) a general analytical solution of the one-dimensional diffusion–reaction equation in porous media, (2) a refined representation of nitrogen inhibition on soil methanotrophy, (3) updated factors governing the influence of soil moisture and temperature on CH4 oxidation rates and (4) the ability to evaluate the impact of autochthonous soil CH4 sources on uptake of atmospheric CH4 . We show that the improved structural and parametric representation of key drivers of soil methanotrophy in MeMo results in a better fit to observational data. A global simulation of soil methanotrophy for the period 1990–2009 using MeMo yielded an average annual sink of 33.5 ± 0.6 Tg CH4 yr −1 . Warm and semi-arid regions (tropical deciduous forest and open shrubland) had the highest CH4 uptake rates of 602 and 518 mg CH4 m −2 yr −1 , respectively. In these regions, favourable annual soil moisture content ( ∼ 20 % saturation) and low seasonal temperature variations (variations ∼ 6 ∘ C) provided optimal conditions for soil methanotrophy and soil–atmosphere gas exchange. In contrast to previous model analyses, but in agreement with recent observational data, MeMo predicted low fluxes in wet tropical regions because of refinements in formulation of the influence of excess soil moisture on methanotrophy. Tundra and mixed forest had the lowest simulated CH4 uptake rates of 176 and 182 mg CH4 m −2 yr −1 , respectively, due to their marked seasonality driven by temperature. Global soil uptake of atmospheric CH4 was decreased by 4 % by the effect of nitrogen inputs to the system; however, the direct addition of fertilizers attenuated the flux by 72 % in regions with high agricultural intensity (i.e. China, India and Europe) and by 4–10 % in agriculture areas receiving low rates of N input (e.g. South America). Globally, nitrogen inputs reduced soil uptake of atmospheric CH4 by 1.38 Tg yr −1 , which is 2–5 times smaller than reported previously. In addition to improved characterization of the contemporary soil sink for atmospheric CH4 , MeMo provides an opportunity to quantify more accurately the relative importance of soil methanotrophy in the global CH4 cycle in the past and its capacity to contribute to reduction of atmospheric CH4 levels under future global change scenarios.

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TL;DR: Surface water characteristics indicate that upwelling of cold, nutrient-rich water from near the seafloor accompanies methane emissions and stimulates CO2 consumption by photosynthesizing phytoplankton, challenging the widely held perception that areas characterized by shallow-water methane seeps and/or strongly elevated sea−air methane flux always increase the global atmospheric greenhouse gas burden.
Abstract: Continued warming of the Arctic Ocean in coming decades is projected to trigger the release of teragrams (1 Tg = 10(6) tons) of methane from thawing subsea permafrost on shallow continental shelves and dissociation of methane hydrate on upper continental slopes. On the shallow shelves (<100 m water depth), methane released from the seafloor may reach the atmosphere and potentially amplify global warming. On the other hand, biological uptake of carbon dioxide (CO2) has the potential to offset the positive warming potential of emitted methane, a process that has not received detailed consideration for these settings. Continuous sea-air gas flux data collected over a shallow ebullitive methane seep field on the Svalbard margin reveal atmospheric CO2 uptake rates (-33,300 ± 7,900 μmol m(-2)⋅d(-1)) twice that of surrounding waters and ∼1,900 times greater than the diffusive sea-air methane efflux (17.3 ± 4.8 μmol m(-2)⋅d(-1)). The negative radiative forcing expected from this CO2 uptake is up to 231 times greater than the positive radiative forcing from the methane emissions. Surface water characteristics (e.g., high dissolved oxygen, high pH, and enrichment of (13)C in CO2) indicate that upwelling of cold, nutrient-rich water from near the seafloor accompanies methane emissions and stimulates CO2 consumption by photosynthesizing phytoplankton. These findings challenge the widely held perception that areas characterized by shallow-water methane seeps and/or strongly elevated sea-air methane flux always increase the global atmospheric greenhouse gas burden.

Journal ArticleDOI
TL;DR: Stable isotope data suggest that biogenic sources are the cause of this emission increase in tropical CH4 emissions during the strong La Niña, and two process-based wetland models predict increases in wetland area consistent with observationally-constrained values, but substantially smaller per-area CH 4 emissions, highlighting the need for improvements in such models.
Abstract: Year-to-year variations in the atmospheric methane (CH4) growth rate show significant correlation with climatic drivers. The second half of 2010 and the first half of 2011 experienced the strongest La Nina since the early 1980s, when global surface networks started monitoring atmospheric CH4 mole fractions. We use these surface measurements, retrievals of column-averaged CH4 mole fractions from GOSAT, new wetland inundation estimates, and atmospheric δ13C-CH4 measurements to estimate the impact of this strong La Nina on the global atmospheric CH4 budget. By performing atmospheric inversions, we find evidence of an increase in tropical CH4 emissions of ∼6-9 TgCH4 yr-1 during this event. Stable isotope data suggest that biogenic sources are the cause of this emission increase. We find a simultaneous expansion of wetland area, driven by the excess precipitation over the Tropical continents during the La Nina. Two process-based wetland models predict increases in wetland area consistent with observationally-constrained values, but substantially smaller per-area CH4 emissions, highlighting the need for improvements in such models. Overall, tropical wetland emissions during the strong La Nina were at least by 5% larger than the long-term mean.

Journal ArticleDOI
TL;DR: Simulating the observed LGM CH4 concentration requires a 46–49% reduction in sources, indicating that the observed amplitude cannot be reconciled, and highlights the need for better understanding of the effects of low CO2 and cooler climate on wetlands and other natural CH4 sources.
Abstract: Atmospheric methane (CH4) varied with climate during the Quaternary, rising from a concentration of 375 p.p.b.v. during the last glacial maximum (LGM) 21,000 years ago, to 680 p.p.b.v. at the beginning of the industrial revolution. However, the causes of this increase remain unclear; proposed hypotheses rely on fluctuations in either the magnitude of CH4 sources or CH4 atmospheric lifetime, or both. Here we use an Earth System model to provide a comprehensive assessment of these competing hypotheses, including estimates of uncertainty. We show that in this model, the global LGM CH4 source was reduced by 28-46%, and the lifetime increased by 2-8%, with a best-estimate LGM CH4 concentration of 463-480 p.p.b.v. Simulating the observed LGM concentration requires a 46-49% reduction in sources, indicating that we cannot reconcile the observed amplitude. This highlights the need for better understanding of the effects of low CO2 and cooler climate on wetlands and other natural CH4 sources.

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TL;DR: In this paper, surface water dissolved methane was sampled at different seasons over a period of 2 years in areas representing a wide range of salinities and anthropogenic impacts in the Yucatan Peninsula, Mexico.
Abstract: Methane concentrations in the water column and emissions to the atmosphere were determined for three tropical coastal lagoons surrounded by mangrove forests on the Yucatan Peninsula, Mexico. Surface water dissolved methane was sampled at different seasons over a period of 2 years in areas representing a wide range of salinities and anthropogenic impacts. The highest surface water methane concentrations (up to 8378 nM) were measured in a polluted canal associated with Terminos Lagoon. In Chelem Lagoon, methane concentrations were typically lower, except in the polluted harbor area (1796 nM). In the relatively pristine Celestun Lagoon, surface water methane concentrations ranged from 41 to 2551 nM. Methane concentrations were negatively correlated with salinity in Celestun, while in Chelem and Terminos high methane concentrations were associated with areas of known pollution inputs, irrespective of salinity. The diffusive methane flux from surface lagoon water to the atmosphere ranged from 0.0023 to 15 mmol CH4 m-2 d-1. Flux chamber measurements revealed that direct methane release as ebullition was up to 3 orders of magnitude greater than measured diffusive flux. Coastal mangrove lagoons may therefore be an important natural source of methane to the atmosphere despite their relatively high salinity. Pollution inputs are likely to substantially enhance this flux. Additional statistically rigorous data collected globally are needed to better consider methane fluxes from mangrove-surrounded coastal areas in response to sea level changes and anthropogenic pollution in order to refine projections of future atmospheric methane budgets.

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TL;DR: In this article, the authors present a comprehensive study showing new results from a shallow gas seep area in 40 m water depth located in the North Sea, Netherlands sector B13 that they call ‘‘Dutch Dogger Bank seeparea.
Abstract: We present a comprehensive study showing new results from a shallow gas seep area in �40 m water depth located in the North Sea, Netherlands sector B13 that we call ‘‘Dutch Dogger Bank seep area.’’ It has been postulated that methane presumably originating from a gas reservoir in �600 m depth below the seafloor is naturally leaking to the seafloor. Our ship-based subbottom echosounder data indicate that the migrating gas is trapped in numerous gas pockets in the shallow sediments. The gas pockets are located at the boundary between the top of the Late Pliocene section and overlying fine-grained sediments, which were deposited during the early Holocene marine transgression after the last glaciation. We mapped gas emissions during three R/V Heincke cruises in 2014, 2015, and 2016 and repeatedly observed up to 850 flares in the study area. Most of them (�80%) were concentrated at five flare clusters. Our repeated analysis revealed spatial similarities of seep clusters, but also heterogeneities in emission intensities. A first calculation of the methane released from these clusters into the water column revealed a flow rate of 277 L/min (SD5140), with two clusters emitting 132 and 142 L/min representing the most significant seepage sites. Above these two flare clusters, elevated methane concentrations were recorded in atmospheric measurements. Our results illustrate the effective transport of methane via gas bubbles through a �40 m water column, and furthermore provide an estimate of the emission rate needed to allow for a contribution to the atmospheric methane concentration.

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TL;DR: In this article, the authors measured changes in CH4 concentration and its isotopic signature by cavity ring-down spectroscopy on chambers containing sediment and plants in the Red Sea and found that CH4 production in all the seagrass stations with an average rate of 85.09 ± 27.80 µmol CH4 m 2 d-1.
Abstract: Atmospheric methane (CH4) is the second strongest greenhouse gas and it is emitted to the atmosphere naturally by different sources. It is crucial to define the dimension of these natural emissions in order to forecast changes in atmospheric CH4 mixing ratio in future scenarios. However, CH4 emissions by seagrass ecosystems in shallow marine coastal systems have been neglected although their global extension. Here we quantify the CH4 production rates of seagrass ecosystems in the Red Sea. We measured changes in CH4 concentration and its isotopic signature by cavity ring-down spectroscopy on chambers containing sediment and plants. We detected CH4 production in all the seagrass stations with an average rate of 85.09 ± 27.80 µmol CH4 m-2 d-1. Our results show that there is no seasonal or daily pattern in the CH4 production rates by seagrass ecosystems in the Red Sea. Taking in account the range of global estimates for seagrass coverage and the average seagrass CH4 production, the global CH4 production and emission by seagrass ecosystems could range from 0.09 to 2.7 Tg yr-1. Because CH4 emission by seagrass ecosystems had not been included in previous global CH4 budgets, our estimate would increase the contribution of marine global emissions, hitherto estimated at 9.1 Tg yr-1, by about 30%. Thus, the potential contribution of seagrass ecosystems to marine CH4 emissions provides sufficient evidence of the relevance of these fluxes as to include seagrass ecosystems in future assessments of the global CH4 budgets.

Journal ArticleDOI
01 Aug 2017-Geoderma
TL;DR: In this paper, the authors analyzed two freshwater and two brackish (oligohaline) marshes in a subtropical estuary, where they assessed methanogenic community structure and abundance by molecular cloning, sequencing, and quantitative PCR methods.

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TL;DR: In this article, a high-sensitivity sensor, combining a multipass cell and wavelength modulation spectroscopy in the near infrared spectral region was designed and implemented for trace gas detection.