Spatial variation in flux, δ<Superscript>13</Superscript>C and δ<Superscript>2</Superscript>H of methane in a small Arctic lake with fringing wetland in western Greenland

Small lakes in northern latitudes represent a significant source of CH₄ to the atmosphere that is predicted to increase with warming in the Arctic. Yet, whole-lake CH₄ budgets are lacking as are measurements of δ¹³C-CH₄ and δ²H-CH₄. In this study, we quantify spatial variability of diffusive and ebullitive fluxes of CH₄ and corresponding δ¹³C-CH₄ and δ²H-CH₄ in a small, Arctic lake system with fringing wetland in southwestern Greenland during summer. Net CH₄ flux was highly variable, ranging from an average flux of 7 mg CH₄ m^?2 d^?1 in the deep-water zone to 154 mg CH₄ m^?2 d^?1 along the lake margin. Diffusive flux accounted for ~8.5 % of mean net CH₄ flux, with plant-mediated and ebullitive flux accounting for the balance of the total net flux. Methane content of emitted ebullition was low (mean ± SD 10 ± 17 %) compared to previous studies from boreal lakes and wetlands. Isotopic composition of net CH₄ emissions varied widely throughout the system, with δ¹³C-CH₄ ranging from ?66.2 to ?55.5 ‰, and δ²H-CH₄ ranging from ?345 to ?258 ‰. Carbon isotope composition of CH₄ in ebullitive flux showed wider variation compared to net flux, ranging from ?69.2 to ?49.2 ‰. Dissolved CH₄ concentrations were highest in the sediment and decreased up the water column. Higher concentrations of CH₄ in the hypoxic deep water coincided with decreasing dissolved O₂ concentrations, while methanotrophic oxidation dominated in the epilimnion based upon decreasing concentrations and increasing values of δ¹³C-CH₄ and δ²H-CH₄. The most depleted ¹³C- and ²H-isotopic values were observed in profundal bottom waters and in subsurface profundal sediments. Based upon paired δ¹³C and δ²H observations of CH₄, acetate fermentation was likely the dominant production pathway throughout the system. However, isotopic ratios of CH₄ in deeper sediments were consistent with mixing/transition between CH₄ production pathways, indicating a higher contribution of the CO₂ reduction pathway. The large spatial variability in fluxes of CH₄ and in isotopic composition of CH₄ throughout a single lake system indicates that the underlying mechanisms controlling CH₄ cycling (production, consumption and transport) are spatially heterogeneous. Net flux along the lake margin dominated whole-lake flux, suggesting the nearshore littoral area dominates CH₄ emissions in these systems. Future studies of whole-lake CH₄ budgets should consider this significant spatial heterogeneity.     

Deep peat warming increases surface methane and carbon dioxide emissions in a black spruce‐dominated ombrotrophic bog

Boreal peatlands contain approximately 500 Pg carbon (C) in the soil, emit globally significant quantities of methane (CH₄), and are highly sensitive to climate change. Warming associated with global climate change is likely to increase the rate of the temperature‐sensitive processes that decompose stored organic carbon and release carbon dioxide (CO₂) and CH₄. Variation in the temperature sensitivity of CO₂ and CH₄ production and increased peat aerobicity due to enhanced growing‐season evapotranspiration may alter the nature of peatland trace gas emission. As CH₄ is a powerful greenhouse gas with 34 times the warming potential of CO₂, it is critical to understand how factors associated with global change will influence surface CO₂ and CH₄ fluxes. Here, we leverage the Spruce and Peatland Responses Under Changing Environments (SPRUCE) climate change manipulation experiment to understand the impact of a 0–9°C gradient in deep belowground warming (“Deep Peat Heat”, DPH) on peat surface CO₂ and CH₄ fluxes. We find that DPH treatments increased both CO₂ and CH₄ emission. Methane production was more sensitive to warming than CO₂ production, decreasing the C‐CO₂:C‐CH₄ of the respired carbon. Methane production is dominated by hydrogenotrophic methanogenesis but deep peat warming increased the δ¹³C of CH₄ suggesting an increasing contribution of acetoclastic methanogenesis to total CH₄ production with warming. Although the total quantity of C emitted from the SPRUCE Bog as CH₄ is <2%, CH₄ represents >50% of seasonal C emissions in the highest‐warming treatments when adjusted for CO₂ equivalents on a 100‐year timescale. These results suggest that warming in boreal regions may increase CH₄ emissions from peatlands and result in a positive feedback to ongoing warming.     

Recovery of Methanogenesis Following Summer Drought in Soils from Two Cool Temperate Peatlands,New York State,USA

Following a summer drought, intact cores of peat soil from two cool temperate peatlands (a rain-fed bog and a groundwater-fed swamp) were exposed experimentally to three different water table levels. The goal was to examine recovery of anaerobic methanogenesis and to evaluate peat soil decomposition to methane (CH₄), carbon dioxide (CO₂), and dissolved organic carbon (DOC) upon rewetting. Methane emission from soils to the atmosphere was greatest (mean = 80 μmol m^?2 s^?1) when the entire peat core was rewetted quickly; emission was negligible at low water level and when peat cores were rewetted gradually. Rates of CO₂ emission (mean = 1.0 μmol m^?2 s^?1) were relatively insensitive to water level. Concentrations of CH₄ in soil air spaces suggest that onset of methanogenesis induces, but later represses, aerobic oxidation of CH₄ above the water table. Concentrations of CO₂ suggest production at the soil surface of swamp peat versus at greater depths in bog peat. Portions of peat soil incubated in vitro without oxygen (O₂) exhibited a lag before the onset of methanogenesis, and the lag time was less in peat from the cores rewetted quickly. The inhibition of methanogenesis by the selective inhibitor 2-bromoethanesulfonic acid (BES) decreased CO₂ production by 20 to 30% but resulted in an increase in concentrations of DOC by 2 to 5 times. The results show that methanogens in peat soils tolerate moderate drought, and recovery varies among different peat types. In peat soils, the inhibition of methanogenesis might enhance DOC availability.     

Regulation of geochemical activity of microorganisms in a petroleum reservoir by injection of H<Subscript>2</Subscript>O<Subscript>2</Subscript> or water-air mixture

In the course of pilot trials of biotechnologies for the enhancement of oil recovery in formation waters of the Gangxi bed of the Dagang oil field (China), microbiological processes were investigated. The biotechnologies are based on injection into the petroleum reservoir of different oxygen sources (H₂O₂ solution or a water-air mixture) with nitrogen and phosphorus salts. The injection of water-air mixture with nitrogen and phosphorus salts resulted in an increase in the number of aerobic and anaerobic organotrophic bacteria, rates of sulfate reduction and methanogenesis in formation water and also the content of CO₂ (from 4.8–12 to 15–23.2%) and methane (from 86–88 to 91.8%) in the gas. The preferential consumption of isotopically light bicarbonate by methanogens resulted in a higher content of the light ¹²C in methane; the δ¹³C/CH₄ value changed from ?45.1…?48.3 to ?50.7…?59.3‰. At the same time, mineral carbonates of the formation water became isotopically heavier; the δ¹³C/Σcarbonates value increased from 3.4…4.0 to 5.4…9.6‰. Growth of hydrocarbon-oxidizing bacteria was accompanied by production of biosurfactants and decreased interfacial tension of formation water. Injection of H₂O₂ solution resulted in the activation of aerobic processes and in suppression of both sulfate reduction and methanogenesis. Methane content in the gas decreased from 86–88 to 75.7–79.8%, probably due to its consumption by methanotrophs. Due to consumption of isotopically light methane, the residual methane carbon became heavier, with the δ¹³C/CH₄ values from ?39.0 to ?44.3‰. At the same time, mineral carbonates of the formation water became isotopically considerably lighter; the δ¹³C/Σcarbonates value decreased from 5.4…9.6 to ?1.4…2.7‰. The additional amount of oil recovered during the trial of both variants of biotechnological treatment was 3819 t.     

Winter precipitation and snow accumulation drive the methane sink or source strength of Arctic tussock tundra

Arctic winter precipitation is projected to increase with global warming, but some areas will experience decreases in snow accumulation. Although Arctic CH₄ emissions may represent a significant climate forcing feedback, long‐term impacts of changes in snow accumulation on CH₄ fluxes remain uncertain. We measured ecosystem CH₄ fluxes and soil CH₄ and CO₂ concentrations and ¹³C composition to investigate the metabolic pathways and transport mechanisms driving moist acidic tundra CH₄ flux over the growing season (Jun–Aug) after 18 years of experimental snow depth increases and decreases. Deeper snow increased soil wetness and warming, reducing soil %O₂ levels and increasing thaw depth. Soil moisture, through changes in soil %O₂ saturation, determined predominance of methanotrophy or methanogenesis, with soil temperature regulating the ecosystem CH₄ sink or source strength. Reduced snow (RS) increased the fraction of oxidized CH₄ (Fox) by 75–120% compared to Ambient, switching the system from a small source to a net CH₄ sink (21 ± 2 and ?31 ± 1 mg CH₄ m^?2 season^?1 at Ambient and RS). Deeper snow reduced Fox by 35–40% and 90–100% in medium‐ (MS) and high‐ (HS) snow additions relative to Ambient, contributing to increasing the CH₄ source strength of moist acidic tundra (464 ± 15 and 3561 ± 97 mg CH₄ m^?2 season^?1 at MS and HS). Decreases in Fox with deeper snow were partly due to increases in plant‐mediated CH₄ transport associated with the expansion of tall graminoids. Deeper snow enhanced CH₄ production within newly thawed soils, responding mainly to soil warming rather than to increases in acetate fermentation expected from thaw‐induced increases in SOC availability. Our results suggest that increased winter precipitation will increase the CH₄ source strength of Arctic tundra, but the resulting positive feedback on climate change will depend on the balance between areas with more or less snow accumulation than they are currently facing.     

Microbial processes influencing methane emission from rice fields

Irrigated rice fields are an important source of atmospheric methane. In order to improve our understanding of the controlling processes, we measured in situ CH₄ emission and CH₄ oxidation in an Italian rice field in 1998 and 1999, and studied CH₄ production in soil and root samples. The CH₄ emission rates were correlated with diurnal temperature variations and showed pronounced seasonal and interannual variations. The contribution of CH₄ oxidation to total CH₄ flux, determined by specific inhibition with difluoromethane, decreased from 40% at the beginning to zero at the end of the season. The stable carbon isotopic composition of the emitted CH₄ also decreased. The CH₄‐oxidizing bacteria probably became limited by nitrogen as indicated by the seasonal decrease of NH₄⁺. Thus, CH₄ oxidation had little effect on CH₄ emission. Methane production on rice roots was relatively constant over the season. Methane production in soil slowly increased after flooding and was highest in the middle of the season. Pore water concentrations of CH₄ showed a similar seasonal pattern. In 1999, CH₄ production increased later in the season and reached lower rates than in 1998. An additional drainage in 1999 resulted in higher ferric iron concentrations, higher soil redox potentials and lower acetate concentrations. As a result, acetate‐utilizing methanogens were probably out‐competed by iron‐reducers so that a larger percentage of [2–¹⁴C]acetate was converted to ¹⁴CO₂ instead of ¹⁴CH₄. The residual CH₄ production was relatively low and was mainly due to H₂/CO₂‐dependent methanogenesis. Experiments with radioactive bicarbonate and with methyl fluoride as specific inhibitor showed that the theoretical ratio of 7:3 of methanogenesis from acetate vs. H₂/CO₂ was only reached later in the season when total CH₄ production was at the maximum. In conclusion, our results give a mechanistic explanation for the intraseasonal and interannual differences in CH₄ emission.     

Suppression of methanogenesis by dissimilatory Fe(III)-reducing bacteria in tropical rain forest soils: implications for ecosystem methane flux

Tropical forests are an important source of atmospheric methane (CH₄), and recent work suggests that CH₄ fluxes from humid tropical environments are driven by variations in CH₄ production, rather than by bacterial CH₄ oxidation. Competition for acetate between methanogenic archaea and Fe(III)‐reducing bacteria is one of the principal controls on CH₄ flux in many Fe‐rich anoxic environments. Upland humid tropical forests are also abundant in Fe and are characterized by high organic matter inputs, steep soil oxygen (O₂) gradients, and fluctuating redox conditions, yielding concomitant methanogenesis and bacterial Fe(III) reduction. However, whether Fe(III)‐reducing bacteria coexist with methanogens or competitively suppress methanogenic acetate use in wet tropical soils is uncertain. To address this question, we conducted a process‐based laboratory experiment to determine if competition for acetate between methanogens and Fe(III)‐reducing bacteria influenced CH₄ production and C isotope composition in humid tropical forest soils. We collected soils from a poor to moderately drained upland rain forest and incubated them with combinations of ¹³C‐bicarbonate, ¹³C‐methyl labeled acetate (¹³CH₃COO^?), poorly crystalline Fe(III), or fluoroacetate. CH₄ production showed a greater proportional increase than Fe²⁺ production after competition for acetate was alleviated, suggesting that Fe(III)‐reducing bacteria were suppressing methanogenesis. Methanogenesis increased by approximately 67 times while Fe²⁺ production only doubled after the addition of ¹³CH₃COO^?. Large increases in both CH₄ and Fe²⁺ production also indicate that the two process were acetate limited, suggesting that acetate may be a key substrate for anoxic carbon (C) metabolism in humid tropical forest soils. C isotope analysis suggests that competition for acetate was not the only factor driving CH₄ production, as ¹³C partitioning did not vary significantly between ¹³CH₃COO^? and ¹³CH₃COO^?+Fe(III) treatments. This suggests that dissimilatory Fe(III)‐reduction suppressed both hydrogenotrophic and aceticlastic methanogenesis. These findings have implications for understanding the CH₄ biogeochemistry of highly weathered wet tropical soils, where CH₄ efflux is driven largely by CH₄ production.     

Stoichiometry and temperature sensitivity of methanogenesis and CO2 production from saturated polygonal tundra in Barrow,Alaska

Arctic permafrost ecosystems store ~50% of global belowground carbon (C) that is vulnerable to increased microbial degradation with warmer active layer temperatures and thawing of the near surface permafrost. We used anoxic laboratory incubations to estimate anaerobic CO₂ production and methanogenesis in active layer (organic and mineral soil horizons) and permafrost samples from center, ridge and trough positions of water‐saturated low‐centered polygon in Barrow Environmental Observatory, Barrow AK, USA. Methane (CH₄) and CO₂ production rates and concentrations were determined at ?2, +4, or +8 °C for 60 day incubation period. Temporal dynamics of CO₂ production and methanogenesis at ?2 °C showed evidence of fundamentally different mechanisms of substrate limitation and inhibited microbial growth at soil water freezing points compared to warmer temperatures. Nonlinear regression better modeled the initial rates and estimates of Q₁₀ values for CO₂ that showed higher sensitivity in the organic‐rich soils of polygon center and trough than the relatively drier ridge soils. Methanogenesis generally exhibited a lag phase in the mineral soils that was significantly longer at ?2 °C in all horizons. Such discontinuity in CH₄ production between ?2 °C and the elevated temperatures (+4 and +8 °C) indicated the insufficient representation of methanogenesis on the basis of Q₁₀ values estimated from both linear and nonlinear models. Production rates for both CH₄ and CO₂ were substantially higher in organic horizons (20% to 40% wt. C) at all temperatures relative to mineral horizons (<20% wt. C). Permafrost horizon (~12% wt. C) produced ~5‐fold less CO₂ than the active layer and negligible CH₄. High concentrations of initial exchangeable Fe(II) and increasing accumulation rates signified the role of iron as terminal electron acceptors for anaerobic C degradation in the mineral horizons.     

Circadian methane oxidation in the root zone of rice plants

In the root zone of rice plants aerobic methanotrophic bacteria catalyze the oxidation of CH₄ to CO₂, thereby reducing CH₄ emissions from paddy soils to the atmosphere. However, methods for in situ quantification of microbial processes in paddy soils are scarce. Here we adapted the push–pull tracer-test (PPT) method to quantify CH₄ oxidation in the root zone of potted rice plants. During a PPT, a test solution containing CH₄ ± O₂ as reactant(s), Cl^? and Ar as nonreactive tracers, and BES as an inhibitor of CH₄ production was injected into the root zone at different times throughout the circadian cycle (daytime, early nighttime, late nighttime). After a 2-h incubation phase, the test solution/pore-water mixture was extracted from the same location and rates of CH₄ oxidation were calculated from the ratio of measured reactant and nonreactive tracer concentrations. In separate rice pots, O₂ concentrations in the vicinity of rice roots were measured throughout the circadian cycle using a fiber-optic sensor. Results indicated highly variable CH₄ oxidation rates following a circadian pattern. Mean rates at daytime and early nighttime varied from 62 up to 451 μmol l^?1 h^?1, whereas at late nighttime CH₄ oxidation rates were low, ranging from 13 to 37 μmol l^?1 h^?1. Similarly, daytime O₂ concentration in the vicinity of rice roots increased to up to 250% air saturation, while nighttime O₂ concentration dropped to below detection (<0.15% air saturation). Our results suggest a functional link between root-zone CH₄ oxidation and photosynthetic O₂ supply.     

Microbial methane cycling in sediments of Arctic thermokarst lagoons

Thermokarst lagoons represent the transition state from a freshwater lacustrine to a marine environment, and receive little attention regarding their role for greenhouse gas production and release in Arctic permafrost landscapes. We studied the fate of methane (CH₄) in sediments of a thermokarst lagoon in comparison to two thermokarst lakes on the Bykovsky Peninsula in northeastern Siberia through the analysis of sediment CH₄ concentrations and isotopic signature, methane-cycling microbial taxa, sediment geochemistry, lipid biomarkers, and network analysis. We assessed how differences in geochemistry between thermokarst lakes and thermokarst lagoons, caused by the infiltration of sulfate-rich marine water, altered the microbial methane-cycling community. Anaerobic sulfate-reducing ANME-2a/2b methanotrophs dominated the sulfate-rich sediments of the lagoon despite its known seasonal alternation between brackish and freshwater inflow and low sulfate concentrations compared to the usual marine ANME habitat. Non-competitive methylotrophic methanogens dominated the methanogenic community of the lakes and the lagoon, independent of differences in porewater chemistry and depth. This potentially contributed to the high CH₄ concentrations observed in all sulfate-poor sediments. CH₄ concentrations in the freshwater-influenced sediments averaged 1.34 ± 0.98 μmol g⁻¹, with highly depleted δ¹³C-CH₄ values ranging from −89‰ to −70‰. In contrast, the sulfate-affected upper 300 cm of the lagoon exhibited low average CH₄ concentrations of 0.011 ± 0.005 μmol g⁻¹ with comparatively enriched δ¹³C-CH₄ values of −54‰ to −37‰ pointing to substantial methane oxidation. Our study shows that lagoon formation specifically supports methane oxidizers and methane oxidation through changes in pore water chemistry, especially sulfate, while methanogens are similar to lake conditions.     

Archaeal Community Structure and Pathway of Methane Formation on Rice Roots

The community structure of methanogenic Archaea on anoxically incubated rice roots was investigated by amplification, sequencing, and phylogenetic analysis of 16S rRNA and methyl-coenzyme M reductase (mcrA) genes. Both genes demonstrated the presence of Methanomicrobiaceae, Methanobacteriaceae, Methanosarcinaceae, Methanosaetaceae, and Rice cluster I, an uncultured methanogenic lineage. The pathway of CH₄ formation was determined from the ¹³C-isotopic signatures of the produced CH₄, CO₂ and acetate. Conditions and duration of incubation clearly affected the methanogenic community structure and the pathway of CH₄ formation. Methane was initially produced from reduction of CO₂ exclusively, resulting in accumulation of millimolar concentrations of acetate. Simultaneously, the relative abundance of the acetoclastic methanogens (Methanosarcinaceae, Methanosaetaceae), as determined by T-RFLP analysis of 16S rRNA genes, was low during the initial phase of CH₄ production. Later on, however, acetate was converted to CH₄ so that about 40% of the produced CH₄ originated from acetate. Most striking was the observed relative increase of a population of Methanosarcina spp. (but not of Methanosaeta spp.) briefly before acetate concentrations started to decrease. Both acetoclastic methanogenesis and Methanosarcina populations were suppressed by high phosphate concentrations, as observed under application of different buffer systems. Our results demonstrate the parallel change of microbial community structure and function in a complex environment, i.e., the increase of acetoclastic Methanosarcina spp. when high acetate concentrations become available.     

Quantitative evaluation of ruminal methane and carbon dioxide formation from formate through C-13 stable isotope analysis in a batch culture system

Methane produced from formate is one of the important methanogensis pathways in the rumen. However, quantitative information of CH₄ production from formate has been rarely reported. The aim of this study was to characterize the conversion rate (CR) of formic acid into CH₄ and CO₂ by rumen microorganisms. Ground lucerne hay was incubated with buffered ruminal fluid for 6, 12, 24 and 48 h. Before the incubation, ¹³C-labeled H¹³COOH was also supplied into the incubation bottle at a dose of 0, 1.5, 2.2 or 2.9 mg/g of DM substrate. There were no interactions (P>0.05) between dose and incubation time for all variables evaluated. When expressed as an absolute amount (ml in gas sample) or a relative CR (%), both ¹³CH₄ and ¹³CO₂ production quadratically increased (P<0.01) with the addition of H¹³COOH. The total ¹³C (¹³CH₄ and ¹³CO₂) CR was also quadratically increased (P<0.01) when H¹³COOH was added. Moreover, formate addition linearly decreased (P<0.031) the concentrations of NH₃-N, total and individual volatile fatty acids (acetate, propionate and butyrate), and quadratically decreased (P<0.014) the populations of protozoa, total methanogens, Methanosphaera stadtmanae, Methanobrevibacter ruminantium M1, Methanobrevibacter smithii and Methanosarcina barkeri. In summary, formate affects ruminal fermentation and methanogenesis, as well as the rumen microbiome, in particular microorganisms which are directly or indirectly involved in ruminal methanogenesis. This study provides quantitative verification for the rapid dissimilation of formate into CH₄ and CO₂ by rumen microorganisms.     

Methanogenic Pathway and Archaeal Community Structure in the Sediment of Eutrophic Lake Dagow: Effect of Temperature

Methanogenic degradation of organic matter is an important microbial process in lake sediments. Temperature may affect not only the rate but also the pathway of CH₄ production by changing the activity and the abundance of individual microorganisms. Therefore, we studied the function and structure of a methanogenic community in anoxic sediment of Lake Dagow, a eutrophic lake in north-eastern Germany. Incubation of sediment samples (in situ 7.5°C) at increasing temperatures (4, 10, 15, 25, 30°C) resulted in increasing production rates of CH₄ and CO₂ and in increasing steady-state concentrations of H₂. Thermodynamic conditions for H₂/CO₂ -dependent methanogenesis were only exergonic at 25 and 30°C. Inhibition of methanogenesis with chloroform resulted in the accumulation of methanogenic precursors, i.e., acetate, propionate, and isobutyrate. Mass balance calculations indicated that less CH₄ was formed via H₂ at 4°C than at 30°C. Conversion of ¹⁴CO₂ to ¹⁴CH₄ also showed that H₂/CO₂ -dependent methanogenesis contributed less to total CH₄ production at 4°C than at 30°C. [2–¹⁴ C]Acetate turnover rates at 4°C accounted for a higher percentage of total CH₄ production than at 30°C. Collectively, these results showed a higher contribution of H₂-dependent methanogenesis and a lower contribution of acetate-dependent methanogenesis at high versus low temperature. The archaeal community was characterized by cloning, sequencing, and phylogenetic analysis of the 16S rRNA genes retrieved from the sediment. Sequences were affiliated with Methanosaetaceae, Methanomicrobiaceae, and three deeply branching euryarchaeotal clusters, i.e., group III, Rice cluster V, and a novel euryarchaeotal cluster, the LDS cluster. Terminal restriction fragment length polymorphism (T-RFLP) analysis showed that 16S rRNA genes affiliated to Methanosaetaceae (20–30%), Methanomicrobiaceae (35–55%), and group III (10–25%) contributed most to the archaeal community. Incubation of the sediment at different temperatures (4–30°C) did not result in a systematic change of the archaeal community composition, indicating that change of temperature primarily affected the activity rather than the structure of the methanogenic community.     

The positive net radiative greenhouse gas forcing of increasing methane emissions from a thawing boreal forest‐wetland landscape

At the southern margin of permafrost in North America, climate change causes widespread permafrost thaw. In boreal lowlands, thawing forested permafrost peat plateaus (‘forest’) lead to expansion of permafrost‐free wetlands (‘wetland’). Expanding wetland area with saturated and warmer organic soils is expected to increase landscape methane (CH₄) emissions. Here, we quantify the thaw‐induced increase in CH₄ emissions for a boreal forest‐wetland landscape in the southern Taiga Plains, Canada, and evaluate its impact on net radiative forcing relative to potential long‐term net carbon dioxide (CO₂) exchange. Using nested wetland and landscape eddy covariance net CH₄ flux measurements in combination with flux footprint modeling, we find that landscape CH₄ emissions increase with increasing wetland‐to‐forest ratio. Landscape CH₄ emissions are most sensitive to this ratio during peak emission periods, when wetland soils are up to 10 °C warmer than forest soils. The cumulative growing season (May–October) wetland CH₄ emission of ~13 g CH₄ m^?2 is the dominating contribution to the landscape CH₄ emission of ~7 g CH₄ m^?2. In contrast, forest contributions to landscape CH₄ emissions appear to be negligible. The rapid wetland expansion of 0.26 ± 0.05% yr^?1 in this region causes an estimated growing season increase of 0.034 ± 0.007 g CH₄ m^?2 yr^?1 in landscape CH₄ emissions. A long‐term net CO₂ uptake of >200 g CO₂ m^?2 yr^?1 is required to offset the positive radiative forcing of increasing CH₄ emissions until the end of the 21st century as indicated by an atmospheric CH₄ and CO₂ concentration model. However, long‐term apparent carbon accumulation rates in similar boreal forest‐wetland landscapes and eddy covariance landscape net CO₂ flux measurements suggest a long‐term net CO₂ uptake between 49 and 157 g CO₂ m^?2 yr^?1. Thus, thaw‐induced CH₄ emission increases likely exert a positive net radiative greenhouse gas forcing through the 21st century.     

Large‐scale patterns in summer diffusive CH4 fluxes across boreal lakes,and contribution to diffusive C emissions

Lakes are a major component of boreal landscapes, and whereas lake CO₂ emissions are recognized as a major component of regional C budgets, there is still much uncertainty associated to lake CH₄ fluxes. Here, we present a large‐scale study of the magnitude and regulation of boreal lake summer diffusive CH₄ fluxes, and their contribution to total lake carbon (C) emissions, based on in situ measurements of concentration and fluxes of CH₄ and CO₂ in 224 lakes across a wide range of lake type and environmental gradients in Québec. The diffusive CH₄ flux was highly variable (mean 11.6 ± 26.4 SD mg m^?2 d^?1), and it was positively correlated with temperature and lake nutrient status, and negatively correlated with lake area and colored dissolved organic matter (CDOM). The relationship between CH₄ and CO₂ concentrations fluxes was weak, suggesting major differences in their respective sources and/or regulation. For example, increasing water temperature leads to higher CH₄ flux but does not significantly affect CO₂ flux, whereas increasing CDOM concentration leads to higher CO₂ flux but lower CH₄ flux. CH₄ contributed to 8 ± 23% to the total lake C emissions (CH₄ + CO₂), but 18 ± 25% to the total flux in terms of atmospheric warming potential, expressed as CO₂‐equivalents. The incorporation of ebullition and plant‐mediated CH₄ fluxes would further increase the importance of lake CH₄. The average Q₁₀ of CH₄ flux was 3.7, once other covarying factors were accounted for, but this apparent Q₁₀ varied with lake morphometry and was higher for shallow lakes. We conclude that global climate change and the resulting shifts in temperature will strongly influence lake CH₄ fluxes across the boreal biome, but these climate effects may be altered by regional patterns in lake morphometry, nutrient status, and browning.     

Methane production in littoral sediment of Lake Constance

Maximum rates of CH₄ production in the littoral sediment were observed in 2–5 cm depth. The CH₄ production rates increased during the year from about 5 mmol m⁻²d⁻¹ in December to a maximum of about 95 mmol m⁻²d⁻¹ in September. CH₄ production rates showed a temperature optimum at 30°C and an apparent activation energy of 76 kJ mol⁻¹. A large part of the seasonality of CH₄ production could be ascribed to the change of the sediment temperature. Most of the produced CH₄ was lost by ebullition. Gas bubbles contained about 60–70% CH₄ with an average δ¹³C of −56.2% and δD of −354%, and 2% CO₂ with an average δ¹³C of −14.1% indicating that CH₄ was produced from methyl carbon, i.e. mainly using acetate as methanogenic substrate. This result was confirmed by inhibition of methanogenesis with chloroform which resulted in an accumulation rate of acetate equivalent to 81% of the rate of CH₄ production. Most probable numbers of methanogenic bacteria were in the order of 10⁴ bacteria g⁻¹d.w. sediment for acetate-, methanol- or formate-utilizing, and of 10⁵ for H₂-utilizing methanogens. The turnover times of acetate were in the order of 2.3–4.8 h which, with in situ acetate concentrations of about 25–50 μM, resulted in rates of acetate turnover which were comparable to the rates of CH₄ production. The respiratory index (RI) showed that [2−¹⁴C]acetate was mainly used by methanogenesis rather than by respiratory processes, although the zone of CH₄ production in the sediment overlapped with the zone of sulfate reduction.     

The fate of <Superscript>13</Superscript>C<Superscript>15</Superscript>N labelled glycine in permafrost and surface soil at simulated thaw in mesocosms from high arctic and subarctic ecosystems

Aims

Poorly drained arctic ecosystems are potential large emitters of methane (CH₄) due to their high soil organic carbon content and low oxygen availability. In wetlands, aerenchymatous plants transport CH₄ from the soil to the atmosphere, but concurrently transport O₂ to the rhizosphere, which may lead to oxidation of CH₄. The importance of the latter process is largely unknown for arctic plant species and ecosystems. Here, we aim to quantify the subsurface oxidation of CH₄ in a waterlogged arctic ecosystem dominated by Carex aquatilis ssp. stans and Eriophorum angustifolium, and evaluate the overall effect of these plants on the CH₄ budget.

Methods

A mesocosms study was established based on the upper 20 cm of an organic soil profile with intact plants retrieved from a peatland in West Greenland (69°N). We measured dissolved concentrations and emissions of ¹³CO₂ and ¹³CH₄ from mesocosms during three weeks after addition of ¹³C-enriched CH₄ below the mesocosm.

Results

Most of the recovered ¹³C label (>98 %) escaped the ecosystem as CH₄, while less than 2 % was oxidized to ¹³CO₂.

Conclusions

It is concluded that aerenchymatous plants control the overall CH₄ emissions but, as a transport system for oxygen, are too inefficient to markedly reduce CH₄ emissions.

     

The carbon and hydrogen stable isotope composition of bacteriogenic methane: A laboratory study using a landfill inoculum

Anaerobic bacterial degradation of landfill waste produces a globally significant source of the greenhouse gas methane. Stable isotopic measurements of methane [δ^I3C(CH₄) and δD(CH₄)] can often fingerprint different sources of methane (natural vs. anthro‐pogenic) and help identify the bacterial processes involved in methane production. Landfill microbial communities are complex and diverse, and hence so too is the biogeochem‐istry of methane formation. To investigate the influence of (l) the methane formation pathway (acetoclastic methanogenesis and CO₂ reduction), and (2) SD of water on the stable isotopic composition of landfill methane, two model butyrate‐degrading landfill systems were established. The systems were inoculated with domestic refuse from a landfill and incubated in the laboratory for 92 days. Both systems were identical except δD of water initially added to system 2 was 118% heavier than system 1. Between days 39 and 72 the systems were resupplemented with butyrate. Production of CH₄ and CO₂ and changes in volatile fatty acid concentration confirmed that active methanogenic populations had been established. CH₄ became ¹³C enriched in both incubations with time. Interpreting changes in acetate, butyrate, and propionate concentration during incubation is complicated, but these observations and other information suggest that the dominant methanogenic substrate changed front CO₂/H₂ to acetate as the experiment progressed. This is also consistent with the observed ¹³C enrichment of CH₄, as ¹³C discrimination during methane production from acetate is less than from CO₂. In contrast, δD(CH₄) remained relatively constant, suggesting that this measurement may not provide a reliable basis for distinguishing between CH₄ from CO₂ reduction and acetoclastic methanogenesis, as has previously been suggested.     

Microbiological and isotopic geochemical investigation of Lake Kislo-Sladkoe,a meromictic water body at the Kandalaksha Bay shore (White Sea)

Microbiological, biogeochemical, and isotopic geochemical investigation of Lake Kislo-Sladkoe (Polusolenoe in early publications) at the Kandalaksha Bay shore (White Sea) was carried out in September 2010. Lake Kislo-Sladkoe was formed in the mid-1900s out of a sea gulf due to a coastal heave. At the time of investigation, the surface layer was saturated with oxygen, while near-bottom water contained sulfide (up to 32 mg/L). Total number of microorganisms was high (12.3 × 10⁶ cells/mL on average). Light CO₂ fixation exhibited two pronounced peaks. In the oxic zone, the highest rates of photosynthesis were detected at 1.0 and 2.0 m. The second, more pronounced peak of light CO₂ fixation was associated with activity of anoxygenic phototrophic bacteria in the anoxic layer at the depth of 2.9 m (413 μg C L^?1 day^?1). Green-colored green sulfur bacteria (GSB) predominated in the upper anoxic layer (2.7–2.9 m), their numbers being as high as 1.12 × 10⁴ cells/mL, while brown-colored GSB predominated in the lower horizons. The rates of both sulfate reduction and methanogenesis peaked in the 2.9 m horizon (1690 μg S L^?1 day^?1 and 2.9 μL CH₄ L^?1 day^-1). The isotopic composition of dissolved methane from the near-bottom water layer (δ¹³C (CH₄) = ?87.76‰) was significantly lighter than in the upper horizons (δ¹³C (CH₄) = ?77.95‰). The most isotopically heavy methane (δ¹³C (CH₄) = ?72.61‰) was retrieved from the depth of 2.9 m. The rate of methane oxidation peaked in the same horizon. As a result of these reactions, organic matter (OM) carbon of the 2.9 m horizon became lighter (?36.36‰), while carbonate carbon became heavier (?7.56‰). Thus, our results demonstrated that Lake Kislo-Sladkoe is a stratified meromictic lake with active microbial cycles of carbon and sulfur. Suspended matter in the water column was mostly of autochthonous origin. Anoxygenic photo-synthesis coupled to utilization of reduced sulfur compounds contributed significantly to OM production.     

Enhanced CH4 emission from a wetland soil exposed to Elevated CO2

Methane emissions from wetland soils are generally a positive function ofplant size and primary productivity, and may be expected to increase dueto enhanced rates of plant growth in a future atmosphere of elevatedCO₂. We performed two experiments with Orontium aquaticum, acommon emergent aquatic macrophyte in temperate and sub-tropical wetlands, todetermine if enhanced rates of photosynthesis in elevated CO₂atmospheres would increase CH₄ emissions from wetland soils.O. aquaticum was grown from seed in soil cores under ambient and elevated(ca. 2-times ambient) concentrations of CO₂ in an initialglasshouse study lasting 3 months and then a growth chamber study lasting 6months. Photosynthetic rates were 54 to 71% higher underelevated CO₂ than ambient CO₂, but plantbiomass was not significantly different at the end of the experiment. Ineach case, CH₄ emissions were higher under elevated thanambient CO₂ levels after 2 to 4 months of treatment, suggestinga close coupling between photosynthesis and methanogenesis in our plant-soilsystem. Methane emissions in the growth chamber study increased by 136%. We observed a significant decrease in transpirationrates under elevated CO₂ in the growth chamber study, andspeculate that elevated CO₂ may also stimulate CH₄ emissions by increasing the extent and duration offlooding in some wetland ecosystems. Elevated CO₂ maydramatically increase CH₄ emissions from wetlands, a sourcethat currently accounts for 40% of global emissions.