Contrasting the paradigm that methane is only produced in anoxic conditions, recent discoveries show that oxic methane production (OMP, aka the methane paradox) occurs in oxygenated surface waters worldwide. OMP drivers and their contribution to global methane emissions, however, are not well constrained. In four adjacent pre-alpine lakes, we determine the net methane production rates in oxic surface waters using two mass balance approaches, accounting for methane sources and sinks. We find that OMP occurs in three out of four studied lakes, often as the dominant source of diffusive methane emissions. Correlations of net methane production versus chlorophyll-a, Secchi and surface mixed layer depths suggest a link with photosynthesis and provides an empirical upscaling approach. As OMP is a methane source in direct contact with the atmosphere, a better understanding of its extent and drivers is necessary to constrain the atmospheric methane contribution by inland waters.
Methane oxidation in lakes removes a large portion of methane (CH4). To date, methane oxidation estimates in lakes have often been derived at low spatial resolution in the water column, preventing understanding of the links to the physicochemical gradients in the stratified regions. We applied a mass balance approach with measured dissolved CH4 and sediment CH4 fluxes to derive high-resolution depth profiles of specific CH4 oxidation rates (kox$$ {k}_{\mathrm{ox}} $$) in the water column during the stratified period of a small eutrophic lake (Soppensee, Switzerland). Estimated kox$$ {k}_{\mathrm{ox}} $$ ranged from 0 to 1 d(-1) and the kox$$ {k}_{\mathrm{ox}} $$ profiles agreed well with previous studies, and were also in agreement with rates from concurrent in situ oxidation experiments. A sensitivity analysis revealed that sediment CH4 flux is the largest source of uncertainty when deriving k(ox). Although previous studies have estimated methane oxidation based on delta C-13(CH4), we showed with numerical modeling that delta C-13(CH4) measurements could not be used to resolve the relative contributions of methane oxidation and sediment fluxes to the water column CH4 balance. Exploration of alternative approaches to derive methane oxidation is needed to reveal potentially unknown or misunderstood drivers of methane oxidation in lakes. The presented mass balance approach has the potential to calculate methane oxidation at high vertical resolution and enhance the spatial limitations of established incubation methods. As methane oxidation is responsible for removing most of the produced methane in lakes, it is as important to accurately resolve the key drivers to predict responses to future climate scenarios.
Abstract Here, we investigate the importance of net CH4 production and emissions in the carbon (C) budget of a small productive lake by monitoring CH4, CO2, and O2 for two consecutive years. During the study period, the lake was mostly a net emitter of both CH4 and CO2, while showing positive net ecosystem production. The analyses suggest that during the whole study period, 32% ± 26% of C produced by net ecosystem production was ultimately converted to CH4 and emitted to the atmosphere. When converted to global warming potential, CH4 emission (in CO2 equivalents) was about 3–10 times higher than CO2 removal from in‐lake net ecosystem production over 100‐yr and 20‐yr time frames, respectively. Although more work in similar systems is needed to generalize these findings, our results provide evidence of the important greenhouse gas imbalance in human‐impacted aquatic systems.
Methane (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.
Atmospheric methane (CH4) concentrations have more than doubled in the past similar to 250 yr, although the sources of this potent greenhouse gas remain poorly constrained. Freshwaters contribute similar to 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.