Ebullition is an important pathway for methane emission from inland waters. However, the mechanisms controlling methane bubble formation and release in aquatic sediments remain unclear. A laboratory incubation experiment was conducted to investigate the dynamics of methane bubble formation, storage, and release in response to hydrostatic head drops in three different types of natural sediment. Homogenized clayey, silty, and sandy sediments (initially quasi‐uniform through the depth of the columns) were incubated in chambers for 3 weeks. We observed three distinct stages of methane bubble formation and release: stage I—microbubble formation‐displacing mobile water from sediment pores with negligible ebullition; stage II—formation of large bubbles, displacing the surrounding sediment with concurrent increase in ebullition; and stage III—formation of conduits with relatively steady ebullition. The maximum depth‐averaged volumetric gas content at steady state varied from 18.8% in clayey to 12.0% in silty and 13.2% in sandy sediment. Gas storage in the sediment columns showed strong vertical stratification: most of the free gas was stored in an upper layer, whose thickness varied with sediment grain size. The magnitude of individual ebullition episodes was linearly correlated to hydrostatic head drop and decreased from clayey to sandy to silty sediment and was in excess of that estimated from gas expansion alone, indicating the release of pore water methane. These findings combined with a hydrodynamic model capable of determining dominant sediment type and depositional zones could help resolve spatial heterogeneities in methane ebullition at medium to larger scales in inland waters.
Large-scale studies are needed to identify the drivers of total mercury (THg) and monomethyl-mercury (MeHg) concentrations in aquatic ecosystems. Studies attempting to link dissolved organic matter (DOM) to levels of THg or MeHg are few and geographically constrained. Additionally, stream and river systems have been understudied as compared to lakes. Hence, the aim of this study was to examine the influence of DOM concentration and composition, morphological descriptors, land uses and water chemistry on THg and MeHg concentrations and the percentage of THg as MeHg (%MeHg) in 29 streams across Europe spanning from 41°N to 64 °N. THg concentrations (0.06-2.78 ng L) were highest in streams characterized by DOM with a high terrestrial soil signature and low nutrient content. MeHg concentrations (7.8-159 pg L) varied non-systematically across systems. Relationships between DOM bulk characteristics and THg and MeHg suggest that while soil derived DOM inputs control THg concentrations, autochthonous DOM (aquatically produced) and the availability of electron acceptors for Hg methylating microorganisms (e.g. sulfate) drive %MeHg and potentially MeHg concentration. Overall, these results highlight the large spatial variability in THg and MeHg concentrations at the European scale, and underscore the importance of DOM composition on mercury cycling in fluvial systems.
Methane bubble formation and transport is an important component of biogeochemical carbon cycling in aquatic sediments. To improve understanding of how sediment mechanical properties influence bubble growth and transport in freshwater sediments, a 20-day laboratory incubation experiment using homogenized natural clay and sand was performed. Methane bubble development at high resolution was characterized by μCT. Initially, capillary invasion by microbubbles (<0.1 mm) dominated bubble formation, with continued gas production (4 days for clay; 8 days for sand), large bubbles formed by deforming the surrounding sediment, leading to enhanced of macropore connectivity in both sediments. Growth of large bubbles (>1 mm) was possible in low shear yield strength sediments (<100 Pa), where excess gas pressure was sufficient to displace the sediment. Lower within the sand, higher shear yield strength (>360 Pa) resulted in a predominance of microbubbles where the required capillary entry pressure was low. Enhanced bubble migration, triggered by a controlled reduction in hydrostatic head, was observed throughout the clay column, while in sand mobile bubbles were restricted to the upper 6 cm. The observed macropore network was the dominant path for bubble movement and release in both sediments.
Abstract. Biogenic methane (CH4) emissions from inland waters contribute substantially to global warming. In aquatic systems, CH4 dissolved in freshwater lakes and reservoirs is highly heterogeneous both in space and time. To better understand the biological and physical processes that affect sources and sinks of CH4 in lakes and reservoirs, dissolved CH4 needs to be measured with a highest temporal resolution. To achieve this goal, we developed the Fast-Response Automated Gas Equilibrator (FaRAGE) for real-time in situ measurement of dissolved CH4 concentration at the water surface and in the water column. FaRAGE can achieve an exceptionally short response time (t95 % = 12 s when including the response time of the gas analyzer) while retaining an equilibration ratio of 63 % and a measurement accuracy of 0.5 %. An equilibration ratio as high as 91.8 % can be reached at the cost of a slightly increased response time (16 s). The FaRAGE is capable of continuously measuring dissolved CH4 concentrations in the nM-to-mM (10−9–10−3 mol L−1) range with a detection limit of sub-nM (10−10 mol L−1), when coupled with a cavity ring-down greenhouse gas analyzer (Picarro GasScouter). It enables the possibility of mapping dissolved CH4 concentration in a quasi three-dimensional manner in lakes. The FaRAGE is simple to operate, inexpensive, and suitable for continuous monitoring with a strong tolerance to suspended particles. The easy adaptability to other gas analyzers such as Ultra-portable Los Gatos and stable isotopic gas analyzer (Picarro G2132-i) also provides the potential for many further applications, e.g. measuring dissolved 13δC-CH4 and CO2.
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