CH4 Dynamics Research Articles

Thaw Transitions and Redox Conditions Drive Methane Oxidation in a Permafrost Peatland

AbstractPermafrost peatlands are a significant source of methane (CH4) emissions to the atmosphere and could emit more CH4 with continued permafrost thaw. Aerobic methane‐oxidizing bacteria may attenuate a substantial fraction of CH4 emissions in thawing permafrost peatlands; however, the impact of permafrost thaw on CH4 oxidation is uncertain. We measured potential CH4 oxidation rates (hereafter, CH4 oxidation) and their predictors using laboratory incubations and in situ porewater redox chemistry across a permafrost thaw gradient of eight thaw stages at Stordalen Mire, a permafrost peatland complex in northernmost Sweden. Methane oxidation rates increased across a gradient of permafrost thaw and differed in transitional thaw stages relative to end‐member stages. Oxidation was consistently higher in submerged fens than in bogs or palsas across a range of CH4 concentrations. We also observed that CH4 oxidation increased with decreasing in situ redox potential and was highest in sites with lower redox potential (Eh < 10 mV) and high water table. Our results suggest that redox potential can be used as an important predictor of CH4 oxidation, especially in thawed permafrost peatlands. Our results also highlight the importance of considering transitional thaw stages when characterizing landscape‐scale CH4 dynamics, because these transitional areas have different rates and controls of CH4 oxidation relative to intact or completely thawed permafrost areas. As permafrost thaw increases the total area of semiwet and wet thaw stages in permafrost peatlands, CH4 oxidation represents an important control on CH4 emissions to the atmosphere.

Methane emissions from fens in Alberta’s boreal region: reference data for functional evaluation of restoration outcomes

The aim of the study was to document methane (CH4) dynamics from fen ecosystems in the Athabasca Oil Sands Region (AOSR) in northern Alberta to create a reference database for evaluation of peatland restoration and reclamation projects in the region. The study included three types of fens commonly occurring in this region: poor fen (open and treed), moderately-rich treed fen, and open saline fen (SF). We quantified CH4 fluxes, pore water concentration (PW[CH4]), and production potential together with ecohydrological variables that may influence CH4 dynamics over four growing seasons. Mean (standard deviation) fluxes for open and treed poor fen [99.8 (269.7) and 68.3 (118.8) mg CH4 m−2 day−1, respectively] were higher than for treed rich [32.8 (63.7) mg CH4 m−2 day−1] and open SFs [34.6 (91.3) mg CH4 m−2 day−1]. The total growing season CH4 emissions from these fens ranged between 3.7 and 11.3 g CH4 m−2. Methane production potential varied from 0.1 (0.1) µmol CH4 g peat−1 day−1 at the SF to 4.6 (0.8) µmol CH4 g peat−1 day−1 at the treed rich fen. The variability of CH4 fluxes and pore water concentration between study sites and years was mostly controlled water table (WT) and soil temperature indicating that these variables should be used to assess the expected CH4 flux in peatland reclamation projects. Large inter-annual variability in CH4 flux illustrates the importance of multi-year records for data used in functional evaluation of restoration outcomes.

Exploring Sources and Biogeochemical Dynamics of Dissolved Methane in the Central Bohai Sea in Summer

To clarify biogeochemical controls of environmental factors on the dynamics of dissolved methane (CH4) in shallow-water coastal oceans, we investigated concentrations, sea-to-air fluxes, and the net cycling rate of CH4 in the central Bohai Sea in summer 2018. During the survey, both summertime stratification and dissolve oxygen deficit were observed. In the surface layer, CH4 concentration ([CH4]) ranged from 3.08 to 10.27 nmol kg−1. The averaged sea-to-air flux was estimated at 6.46 ± 3.32mol m−2 d−1, supporting that the Bohai Sea serves as a source of atmospheric CH4. In the bottom layer, [CH4] ranged from 4.29 to 31.04 nmol kg−1. The downward increase of [CH4] within water column indicated substantial sources of CH4 from seafloor. Based on the complex relationship between saturation ratio of CH4 and dissolved oxygen, three types of CH4 release from the seafloor were identified, including diagenesis of buried organic matters, natural leakage from geological settings, and anthropogenic release from offshore oil/gas development. Saturation ratios of CH4 in bottom waters were positively correlated with stratification degree of the water column. Using a two-layer box model, sedimentary CH4 release rates at two oxygen-deficient stations were estimated to be 56.0–60.8 mol m−2 d−1, which were much higher than the sea-to-air fluxes. The modeling results also indicated that the majority of seafloor released CH4 (> 90%) was consumed in the water column of this shallow-water coastal sea. This is the first comprehensive study on CH4 cycling in the Bohai Sea. This work shows the indicating role of dissolved oxygen in identifying multiple CH4 sources and highlights the dominating effects of water stratification and microbial consumption on local CH4 dynamics.

The benthic foraminiferal \u03b434S records flux and timing of paleo methane emissions

In modern environments, pore water geochemistry and modelling simulations allow the study of methane (CH4) sources and sinks at any geographic location. However, reconstructing CH4 dynamics in geological records is challenging. Here, we show that the benthic foraminiferal δ34S can be used to reconstruct the flux (i.e., diffusive vs. advective) and timing of CH4 emissions in fossil records. We measured the δ34S of Cassidulina neoteretis specimens from selected samples collected at Vestnesa Ridge, a methane cold seep site in the Arctic Ocean. Our results show lower benthic foraminiferal δ34S values (∼20‰) in the sample characterized by seawater conditions, whereas higher values (∼25–27‰) were measured in deeper samples as a consequence of the presence of past sulphate-methane transition zones. The correlation between δ34S and the bulk benthic foraminiferal δ13C supports this interpretation, whereas the foraminiferal δ18O-δ34S correlation indicates CH4 advection at the studied site during the Early Holocene and the Younger-Dryas – post-Bølling. This study highlights the potential of the benthic foraminiferal δ34S as a novel tool to reconstruct the flux of CH4 emissions in geological records and to indirectly date fossil seeps.

Sediment Properties Drive Spatial Variability of Potential Methane Production and Oxidation in Small Streams

AbstractEmissions of the potent greenhouse gas methane (CH4) from streams and rivers are a significant component of global freshwater methane emissions. The distribution of CH4 production and oxidation within stream sections and in vertical sediment profiles is not well understood, and the environmental controls on CH4 production and emission in such systems create a significant challenge for assessing larger‐scale dynamics. Here we investigate factors driving the spatial variability of sediment potential methane production (PMP) and potential methane oxidation (PMO) in a temperate stream network in Germany. PMP was highly variable, ranging from 5 × 10−4 to 28.58 μg CH4 gDW−1 d−1 and PMO ranged from 0.43 μg CH4 gDW−1 d−1 to 14.41 μg CH4 gDW−1 d−1. Important drivers of spatial variability of PMP and PMO in the sediments of the stream main‐stem were related to fine sediment fraction and organic carbon content. At smaller spatial scale, that is, in a sub‐catchment stream section, the drivers were more complex and included sediment nitrogen and organic carbon content, as well as porewater dissolved organic carbon, dissolved organic matter quality, and metal concentrations. As with reservoirs and impounded rivers, fine sediment deposition and organic carbon content were found to be key controls on the spatial variability of CH4 production and oxidation. These findings enhance our understanding of CH4 dynamics, improve the potential for identifying CH4 production hotspots in small streams, and provide a potential means for upscaling emission rates in larger‐scale assessments.

Magnitude and Drivers of Potential Methane Oxidation and Production across the Tibetan Alpine Permafrost Region

Methane (CH4) dynamics across permafrost regions is critical in determining the magnitude and direction of permafrost carbon (C)-climate feedback. However, current studies are mainly derived from the Arctic area, with limited evidence from other permafrost regions. By combining large-scale laboratory incubation across 51 sampling sites with machine learning techniques and bootstrap analysis, here, we determined regional patterns and dominant drivers of CH4 oxidation potential in alpine steppe and meadow (CH4 sink areas) and CH4 production potential in swamp meadow (CH4 source areas) across the Tibetan alpine permafrost region. Our results showed that both CH4 oxidation potential (in alpine steppe and meadow) and CH4 production potential (in swamp meadow) exhibited large variability across various sampling sites, with the median value being 8.7, 9.6, and 11.5 ng g-1 dry soil h-1, respectively. Our results also revealed that methanotroph abundance and soil moisture were two dominant factors regulating CH4 oxidation potential, whereas CH4 production potential was mainly affected by methanogen abundance and the soil organic carbon content, with functional gene abundance acting as the best explaining variable. These results highlight the crucial role of microbes in regulating CH4 dynamics, which should be considered when predicting the permafrost C cycle under future climate scenarios.

Methane Production Pathway Regulated Proximally by Substrate Availability and Distally by Temperature in a High‐Latitude Mire Complex

AbstractProjected 21st century changes in high‐latitude climate are expected to have significant impacts on permafrost thaw, which could cause substantial increases in emissions to the atmosphere of carbon dioxide (CO2) and methane (CH4, which has a global warming potential 28 times larger than CO2 over a 100‐year horizon). However, predicted CH4 emission rates are very uncertain due to difficulties in modeling complex interactions among hydrological, thermal, biogeochemical, and plant processes. Methanogenic production pathways (i.e., acetoclastic [AM] and hydrogenotrophic [HM]) and the magnitude of CH4 emissions may both change as permafrost thaws, but a mechanistic analysis of controls on such shifts in CH4 dynamics is lacking. In this study, we reproduced observed shifts in CH4 emissions and production pathways with a comprehensive biogeochemical model (ecosys) at the Stordalen Mire in subarctic Sweden. Our results demonstrate that soil temperature changes differently affect AM and HM substrate availability, which regulates magnitudes of AM, HM, and thereby net CH4 emissions. We predict very large landscape‐scale, vertical, and temporal variations in the modeled HM fraction, highlighting that measurement strategies for metrics that compare CH4 production pathways could benefit from model informed scale of temporal and spatial variance. Finally, our findings suggest that the warming and wetting trends projected in northern peatlands could enhance peatland AM fraction and CH4 emissions even without further permafrost degradation.

The influence of Carex aquatilis and Juncus balticus on methane dynamics: A comparison with water sourced from a natural and a constructed fen

As fen peatlands have been heavily disturbed by resource extraction in northeastern Alberta, Canada, fen construction has been completed. In order to optimize biogeochemical function of future constructed fens, it is beneficial to understand methane (CH4) cycling of newly constructed fens, and how revegetation strategies influence CH4 dynamics. Here, we investigate the effects of two vascular species used for fen construction on CH4 dynamics. A factorial greenhouse experiment using peat columns and a laboratory incubation experiment were used to understand differences in CH4 production, emissions, pore water concentration, and oxidation between Carex aquatilis Wahlenb. and Juncus balticus Willd. The experiment also considered how water sourced from the constructed fen influenced CH4 dynamics compared to natural rich fen water. Higher pore water CH4 concentration and potential CH4 production were found at C. aquatilis columns, possibly associated with higher labile carbon throughout the column. In columns with J. balticus, evidence to support radial oxygen loss reducing CH4 concentration and production was found. Water sampled from peat columns with constructed fen water had higher Fe (all cation forms), Mn (all cation forms), SO42−, and NO3− compared to columns with rich fen water, which corresponded to lower CH4 emissions and pore water concentration. Results from this study could be used to inform revegetation designs of future constructed fens that consider greenhouse gas emissions, including CH4, as a reclamation goal.

The ratio of methanogens to methanotrophs and water-level dynamics drive methane transfer velocity in a temperate kettle-hole peat bog

Abstract. Peatlands are a large source of methane (CH4) to the atmosphere, yet the uncertainty around the estimates of CH4 flux from peatlands is large. To better understand the spatial heterogeneity in temperate peatland CH4 emissions and their response to physical and biological drivers, we studied CH4 dynamics throughout the growing seasons of 2017 and 2018 in Flatiron Lake Bog, a kettle-hole peat bog in Ohio. The site is composed of six different hydro-biological zones: an open water zone, four concentric vegetation zones surrounding the open water, and a restored zone connected to the main bog by a narrow channel. At each of these locations, we monitored water level (WL), CH4 pore-water concentration at different peat depths, CH4 fluxes from the ground and from representative plant species using chambers, and microbial community composition with a focus here on known methanogens and methanotrophs. Integrated CH4 emissions for the growing season were estimated as 315.4±166 mgCH4m-2d-1 in 2017 and 362.3±687 mgCH4m-2d-1 in 2018. Median CH4 emission was highest in the open water, then it decreased and became more variable through the concentric vegetation zones as the WL dropped, with extreme emission hotspots observed in the tamarack mixed woodlands (Tamarack) and low emissions in the restored zone (18.8–30.3 mgCH4m-2d-1). Generally, CH4 flux from above-ground vegetation was negligible compared to ground flux (<0.4 %), although blueberry plants were a small CH4 sink. Pore-water CH4 concentrations varied significantly among zones, with the highest values in the Tamarack zone, close to saturation, and the lowest values in the restored zone. While the CH4 fluxes and pore-water concentrations were not correlated with methanogen relative abundance, the ratio of methanogens to methanotrophs in the upper portion of the peat was significantly correlated to CH4 transfer velocity (the CH4 flux divided by the difference in CH4 pore-water concentration between the top of the peat profile and the concentration in equilibrium with the atmosphere). Since ebullition and plant-mediated transport were not important sources of CH4 and the peat structure and porosity were similar across the different zones in the bog, we conclude that the differences in CH4 transfer velocities, and thus the flux, are driven by the ratio of methanogen to methanotroph relative abundance close to the surface. This study illustrates the importance of the interactions between water-level and microbial composition to better understand CH4 fluxes from bogs and wetlands in general.

High-resolution underwater laser spectrometer sensing provides new insights into methane distribution at an Arctic seepage site

Abstract. Methane (CH4) in marine sediments has the potential to contribute to changes in the ocean and climate system. Physical and biochemical processes that are difficult to quantify with current standard methods such as acoustic surveys and discrete sampling govern the distribution of dissolved CH4 in oceans and lakes. Detailed observations of aquatic CH4 concentrations are required for a better understanding of CH4 dynamics in the water column, how it can affect lake and ocean acidification, the chemosynthetic ecosystem, and mixing ratios of atmospheric climate gases. Here we present pioneering high-resolution in situ measurements of dissolved CH4 throughout the water column over a 400 m deep CH4 seepage area at the continental slope west of Svalbard. A new fast-response underwater membrane-inlet laser spectrometer sensor demonstrates technological advances and breakthroughs for ocean measurements. We reveal decametre-scale variations in dissolved CH4 concentrations over the CH4 seepage zone. Previous studies could not resolve such heterogeneity in the area, assumed a smoother distribution, and therefore lacked both details on and insights into ongoing processes. We show good repeatability of the instrument measurements, which are also in agreement with discrete sampling. New numerical models, based on acoustically evidenced free gas emissions from the seafloor, support the observed heterogeneity and CH4 inventory. We identified sources of CH4, undetectable with echo sounder, and rapid diffusion of dissolved CH4 away from the sources. Results from the continuous ocean laser-spectrometer measurements, supported by modelling, improve our understanding of CH4 fluxes and related physical processes over Arctic CH4 degassing regions.

Methane formation and consumption by sediments in a cross-channel profile of a small river impoundment

Rivers are a natural source of methane (CH4) into the atmosphere and may contribute significantly to total CH4 emissions. Even though the details of sources of CH4 in rivers are not fully understood, weirs have been recognized as a hotspot of CH4 emissions. In this study, we investigated CH4 production and consumption in air-exposed river sediments along a cross-channel transect located upstream of a weir. Stable carbon isotopes were used for determination of individual methanogenic pathways. In order to understand the relationship between physicochemical and biological processes, additional parameters such as organic matter, grain median size, and carbon and nitrogen content were characterized as well. Generally, samples from the surface sediment layer (0-10 cm) had higher CH4 production than sediments from the deeper layer (10-20 cm) during the incubation experiments. Sediments near the bank zones and in the mid-channel were characterized by the highest organic carbon content (6.9 %) as well the highest methanogenic activity (2.5 mmol g-1 DW d-1). The CH4 production was predominated by H2/CO2 dependent methanogenesis in the surface sediment layer (0-10 cm), while the proportion of acetoclastic and hydrogenotrophic methanogenesis in the deeper sediment layer (10-20 cm) was balanced. The CH4 oxidation potential of sediments showed the same spatial pattern as observed for the CH4 production. Our results showed high spatial variability of sediment CH4 production and oxidation in the cross-channel profile upstream of the weir, whereas the highest CH4 dynamics were observed in the littoral zones. This variability was closely linked with the carbon and nitrogen content in the sediment samples.

Radiative forcing of methane fluxes offsets net carbon dioxide uptake for a tropical flooded forest.

Wetlands are important sources of methane (CH4 ) and sinks of carbon dioxide (CO2 ). However, little is known about CH4 and CO2 fluxes and dynamics of seasonally flooded tropical forests of South America in relation to local carbon (C) balances and atmospheric exchange. We measured net ecosystem fluxes of CH4 and CO2 in the Pantanal over 2014-2017 using tower-based eddy covariance along with C measurements in soil, biomass and water. Our data indicate that seasonally flooded tropical forests are potentially large sinks for CO2 but strong sources of CH4 , particularly during inundation when reducing conditions in soils increase CH4 production and limit CO2 release. During inundation when soils were anaerobic, the flooded forest emitted 0.11±0.002g CH4 -Cm-2 d-1 and absorbed 1.6±0.2gCO2 -Cm-2 d-1 (mean±95% confidence interval for the entire study period). Following the recession of floodwaters, soils rapidly became aerobic and CH4 emissions decreased significantly (0.002±0.001gCH4 -Cm-2 d-1 ) but remained a net source, while the net CO2 flux flipped from being a net sink during anaerobic periods to acting as a source during aerobic periods. CH4 fluxes were 50 times higher in the wet season; DOC was a minor component in the net ecosystem carbon balance. Daily fluxes of CO2 and CH4 were similar in all years for each season, but annual net fluxes varied primarily in relation to flood duration. While the ecosystem was a net C sink on an annual basis (absorbing 218gCm-2 (as CH4 -C+CO2 -C) in anaerobic phases and emitting 76gCm-2 in aerobic phases), high CH4 effluxes during the anaerobic flooded phase and modest CH4 effluxes during the aerobic phase indicate that seasonally flooded tropical forests can be a net source of radiative forcings on an annual basis, thus acting as an amplifying feedback on global warming.

Influence of water column stratification and mixing patterns on the fate of methane produced in deep sediments of a small eutrophic lake

AbstractMethane (CH4), a potent greenhouse gas, is produced in and emitted from lakes at globally significant rates. The drivers controlling the proportion of produced CH4 that will reach the atmosphere, however, are still not well understood. We sampled a small eutrophic lake (Soppensee, Switzerland) in 2016–2017 for CH4 concentrations profiles and emissions, combined with water column hydrodynamics to investigate the fate of CH4 produced in hypolimnetic sediments. Using a mass balance approach for the periods between April and October of both years, net CH4 production rates in hypolimnetic sediments ranged between 11.4 and 17.7 mmol m−2 d−1, of which 66–88% was stored in the hypolimnion, 13–27% was diffused to the epilimnion, and 6–7% left the sediments via ebullition. Combining these results with a process‐based model we show that water column turbulent diffusivity (K z) had a major influence on the fate of produced CH4 in the sediments, where higher K z values potentially lead to greater proportion being oxidized and lower K z lead to a greater proportion being stored. During fall when the water column mixes, we found that a greater proportion of stored CH4 is emitted if the lake mixes rapidly, whereas a greater proportion will be oxidized if the water column mixes more gradually. This work highlights the central role of lake hydrodynamics in regulating CH4 dynamics and further suggests the potential for CH4 production and emissions to be sensitive to climate‐driven alterations in lake mixing regimes and stratification.

Kinetics of organic carbon mineralization and methane formation in marine sediments (Aarhus Bay, Denmark)

Abstract Sediments were sampled at nine stations on a transect across a 7–10 m thick Holocene mud layer in Aarhus Bay, Denmark, to investigate the linkages between CH4 dynamics and the rate and depth distribution of organic matter degradation. High-resolution sulfate reduction rates determined by tracer experiments (35S-SRR) decreased by several orders of magnitude down through the mud layer. The rates showed a power law dependency on sediment age: SRR (nmol cm−3 d−1) = 106.18 × Age−2.17. The rate data were used to independently quantify enhanced SO42− transport by bioirrigation. Field data (SO42–, TCO2, T13CO2, NH4+ and CH4 concentrations) could be simulated with a reaction-transport model using the derived bioirrigation rates and assuming that the power law was continuous into the methanogenic sediments below the sulfate-methane transition zone (SMTZ). The model predicted an increase in anaerobic organic carbon mineralization rates across the transect from 2410 to 3540 nmol C cm−2 d−1 caused by an increase in the sediment accumulation rate. Although methanogenesis accounted for only ∼1% of carbon mineralization, a large relative increase in methanogenesis along the transect led to a considerable shallowing of the SMTZ from 428 to 257 cm. Methane gas bubbles appeared once a threshold in the sedimentation accumulation rate was surpassed. The 35S-measured SRR data indicated active sulfate reduction throughout the SO42− zone whereas quasi-linear SO42− gradients over the same zone indicated insignificant sulfate reduction. This apparent inconsistency, observed at all stations, was reconciled by considering the transport of SO42− into the sediment by bioirrigation, which accounted for 94 ± 2% of the total SO42− flux across the sediment-water interface. The SRR determined from the quasi-linear SO42− gradients were two orders of magnitude lower than measured rates. We conclude that models solely based on SO42− concentration gradients will not capture high SRRs at the top of the sulfate reduction zone if they do not properly account for (i) SO42− influx by bioirrigation, and/or (ii) the continuity of organic matter reactivity with sediment depth or age.

Methane Emissions From the Salt Marshes of Doñana Wetlands: Spatio-Temporal Variability and Controlling Factors

Coastal wetlands are significant sources of methane to the atmosphere, but emissions in these ecosystems are still poorly quantified, as in situ data are limited. In this study, we present the first assessment of spatio-temporal changes in air-water CH4 fluxes in the salt marshes of Donana wetlands (SW Spain), one of the most emblematic protected areas in Europe due to its high biotic diversity and unique importance for aquatic wildfowl. The marshes are flooded by estuarine waters from the adjacent Guadalquivir River by tidal intrusion, which must influence aquatic CH4 dynamics through changes in salinity and water chemistry that affects sedimentary methanogenesis. During sixteen samplings conducted between March 2016 and March 2018, surface water CH4 concentrations were measured by using static-head space equilibration gas chromatography in seven sites representing salt marshes located in the land strip close to the estuary. Because of meteorological conditions and tide variations, salinity markedly changed across the salt marshes, although sites located closer to the river mouth could be categorized as polyhaline marshes whereas upstream sites formed a group of mesohaline marshes. The CH4 saturation range was 252-36,735 % (average 5,170%) and 374-620,007 % (average 31,541%) in polyhaline and mesohaline marshes respectively, suggesting inhibitory effect of sulfate on methanogenesis, although a linear trend between dissolved CH4 concentration and salinity was not observed. In contrast, water temperature and chlorophyll a were significantly and positively correlated with methane, indicating sedimentary methanogenesis control by temperature and organic matter availability boosted by primary productivity. This does not exclude the possibility that some CH4 might come from estuarine inputs. Air-water CH4 fluxes ranged from 2.6 to 720 μmol m−2d−1 (average 104 μmol m−2 d−1) in the polyhaline marshes and from 5.6 to 12,715 μmol m−2d−1 (average 637 μmol m−2 d−1) in the mesohaline marshes, with the higher emissions being measured during the summer months in all sites. Even though the strongest environmental drivers of dissolved CH4 accumulation seemed to be temperature and productivity, the spatio-temporal patterns observed suggest that methane dynamics in Donana salt marshes are controlled by a mosaic of processes rather than by a single environmental force.

Methane dynamics in the subsaline ponds of the Chihuahuan Desert: A first assessment

The Cuatro Cienegas Basin (CCB) in the Chihuahuan desert is characterized by the presence of over 500 ponds located in an endorheic basin. These ponds are subsaline ecosystems characterized by a low productivity and a particularly high sulfate concentration, comparable to marine environments. This study focused on assessing the main physicochemical parameters in these ponds along with the characterization of the CH4 dynamics through the determination of fluxes, dissolved CH4 concentrations, and net methanotrophic and methanogenic activity. Despite a sulfate concentration ranging from 1.06 to 4.73 g L−1, the studied ponds showed moderate but clear CH4 production and emission, which suggests that methanogenesis is not completely outcompeted by sulfate reduction. CH4 fluxes ranged from 0.12 to 0.98 mg m−2 d−1, which falls within the higher range of marine emissions and within the lower range reported for coastal saline lagoons and saline ponds. During summer, significant CH4 production in the oxic water column was observed. In addition to CH4, CO2 fluxes were determined at levels from 0.2 to 53 g m−2 d−1, which is within the range recorded for saline lakes in other parts of the world. Our results provide additional evidence that subsaline/saline aquatic ecosystems play an important role in the emission of greenhouse gases to the atmosphere.

Multi-year effect of wetting on CH<sub>4</sub> flux at taiga–tundra boundary in northeastern Siberia deduced from stable isotope ratios of CH<sub>4</sub>

Abstract. The response of CH4 emission from natural wetlands due to meteorological conditions is important because of its strong greenhouse effect. To understand the relationship between CH4 flux and wetting, we observed interannual variations in chamber CH4 flux, as well as the concentration, δ13C, and δD of dissolved CH4 during the summer from 2009 to 2013 at the taiga–tundra boundary in the vicinity of Chokurdakh (70∘37′ N, 147∘55′ E), located on the lowlands of the Indigirka River in northeastern Siberia. We also conducted soil incubation experiments to interpret δ13C and δD of dissolved CH4 and to investigate variations in CH4 production and oxidation processes. Methane flux showed large interannual variations in wet areas of sphagnum mosses and sedges (36–140 mg CH4 m−2 day−1 emitted). Increased CH4 emission was recorded in the summer of 2011 when a wetting event with extreme precipitation occurred. Although water level decreased from 2011 to 2013, CH4 emission remained relatively high in 2012, and increased further in 2013. Thaw depth became deeper from 2011 to 2013, which may partly explain the increase in CH4 emission. Moreover, dissolved CH4 concentration rose sharply by 1 order of magnitude from 2011 to 2012, and increased further from 2012 to 2013. Large variations in δ13C and δD of dissolved CH4 were observed in 2011, and smaller variations were seen in 2012 and 2013, suggesting both enhancement of CH4 production and less significance of CH4 oxidation relative to the larger pool of dissolved CH4. These multi-year effects of wetting on CH4 dynamics may have been caused by continued soil reduction across multiple years following the wetting. Delayed activation of acetoclastic methanogenesis following soil reduction could also have contributed to the enhancement of CH4 production. These processes suggest that duration of water saturation in the active layer can be important for predicting CH4 emission following a wetting event in the permafrost ecosystem.

Sources and sinks of CO2 and CH4 in siliciclastic subterranean estuaries

AbstractAnthropogenic production of greenhouse gases (GHGs) has intensified the need to constrain estimates of natural atmospheric sources from both terrestrial and marine systems. Estuaries are known sources of carbon dioxide (CO2) and methane (CH4); however, less is known about GHG dynamics in subterranean estuaries (STEs). We evaluate CO2 and CH4 dynamics in three proximal STEs bordering Indian River Lagoon, Florida, where groundwater flows through siliciclastic sediments with minor carbonate mineral contents. Although the three STEs have similar mineralogical and flow characteristics, CO2 and CH4 concentrations vary by orders of magnitude. Nonconservative mixing of both gases is observed, and CH4 is generally produced while CO2 is sequestered. The extent of methanogenesis is linked to the redox potential of inflowing groundwaters, as well as degree of CH4 oxidation, which results mostly from anaerobic oxidation of methane. Methane concentrations vary by orders of magnitude, and stable isotopic signatures suggest differences in the microbial production pathway between sites. CO2 is sequestered due to the production of alkalinity relative to dissolved inorganic carbon, which occurs both through rapid CaCO3 dissolution at the shoreline as low‐pH groundwater from the siliciclastic aquifer interacts with carbonate minerals in lagoon sediments, as well as redox reactions, particularly sulfate reduction and denitrification. These results demonstrate a high variability in CO2 and CH4 concentrations, and thus fluxes, even among geographically constrained and hydrogeologically similar STEs. Although STEs are sources of both CO2 and CH4 to surface waters, the variability of production and consumption complicates global estimates of GHG fluxes from STEs.

What the bubble knows: Lake methane dynamics revealed by sediment gas bubble composition

AbstractAtmospheric methane (CH4) concentrations have more than doubled in the past ~ 250 yr, although the sources of this potent greenhouse gas remain poorly constrained. Freshwaters contribute ~ 20% of natural CH4 emissions, about half attributed to ebullition. Estimates remain uncertain as ebullition is stochastic, making measurements difficult, time consuming, and costly with current methods (e.g., floating chambers, funnel gas traps, and hydroacoustics). We present a novel approach to quantify basin‐wide hypolimnetic CH4 fluxes at the sediment level based on measurements of bubble gas content and modeling of dissolved pore‐water gases. We show that the relative ebullition flux pathway can be resolved by knowledge of only bubble gas content. As sediment CH4 production, diffusion, and ebullition are interrelated, the addition of a second observation allows closing the entire sediment CH4 balance. Such measurements could include bubble formation depth, sediment diffusive fluxes, ebullition, sediment CH4 production, or the hypolimnetic CH4 mass balance. The measurement of bubble gas content is particularly useful for identifying local ebullitive hotspots and integrating spatial heterogeneity of CH4 fluxes. Our results further revealed the crucial effect of water column depth, production rates, and hypolimnetic dissolved CH4 concentrations on sediment CH4 dynamics. Although we apply the model to cohesive sediments in an anoxic hypolimnion, the model can be applied to shallow, oxic settings by altering the CH4 production rate curve to account for oxidation. Utilizing our approach will provide a deeper understanding of in‐lake CH4 budgets, and thus improve CH4 emission estimates from inland freshwaters at the regional and global scales.

Zero to moderate methane emissions in a densely rooted, pristine Patagonian bog – biogeochemical controls as revealed from isotopic evidence

Abstract. Peatlands are significant global methane (CH4) sources, but processes governing CH4 dynamics have been predominantly studied in the Northern Hemisphere. Southern hemispheric and tropical bogs can be dominated by cushion-forming vascular plants (e.g. Astelia pumila, Donatia fascicularis). These cushion bogs are found in many (mostly southern) parts of the world but could also serve as extreme examples for densely rooted northern hemispheric bogs dominated by rushes and sedges. We report highly variable summer CH4 emissions from different microforms in a Patagonian cushion bog as determined by chamber measurements. Driving biogeochemical processes were identified from pore water profiles and carbon isotopic signatures. Intensive root activity throughout a rhizosphere stretching over 2 m in depth accompanied by molecular oxygen release created aerobic microsites in water-saturated peat, leading to a thorough CH4 oxidation (< 0.003 mmol L−1 pore water CH4, enriched in δ13C-CH4 by up to 10 ‰) and negligible emissions (0.09±0.16 mmol CH4 m−2 d−1) from Astelia lawns. In sparsely or even non-rooted peat below adjacent pools pore water profile patterns similar to those obtained under Astelia lawns, which emitted very small amounts of CH4 (0.23±0.25 mmol m−2 d−1), were found. Below the A. pumila rhizosphere pore water concentrations increased sharply to 0.40±0.25 mmol CH4 L−1 and CH4 was predominantly produced by hydrogenotrophic methanogenesis. A few Sphagnum lawns and – surprisingly – one lawn dominated by cushion-forming D. fascicularis were found to be local CH4 emission hotspots with up to 1.52±1.10 mmol CH4 m−2 d−1 presumably as root density and molecular oxygen release dropped below a certain threshold. The spatial distribution of root characteristics supposedly causing such a pronounced CH4 emission pattern was evaluated on a conceptual level aiming to exemplify scenarios in densely rooted bogs. We conclude that presence of cushion vegetation as a proxy for negligible CH4 emissions from cushion bogs needs to be interpreted with caution. Nevertheless, overall ecosystem CH4 emissions at our study site were probably minute compared to bog ecosystems worldwide and widely decoupled from environmental controls due to intensive root activity of A. pumila, for example.