Browsing by Author "Einsiedl, Florian"
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Item Open Access Biogeochemical evidence of anaerobic methane oxidation and anaerobic ammonium oxidation in a stratified lake using stable isotopes(Copernicus Publications, 2020-10-23) Einsiedl, Florian; Wunderlich, Anja; Sebilo, Mathieu; Coskun, Ömer K.; Orsi, William D.; Mayer, BernhardNitrate pollution of freshwaters and methane emissions into the atmosphere are crucial factors in deteriorating the quality of drinking water and in contributing to global climate change. The n-damo (nitrite-dependent anaerobic methane oxidation), nitrate-dependent anaerobic methane oxidation and the anaerobic oxidation of ammonium (anammox) represent two microbially mediated processes that can reduce nitrogen loading of aquatic ecosystems and associated methane emissions to the atmosphere. Here, we report vertical concentration and stable-isotope profiles of CH4, NO−3, NO−2, and NH+4 in the water column of Fohnsee (lake in southern Bavaria, Germany) that may indicate linkages between denitrification, anaerobic oxidation of methane (AOM), and anammox. At a water depth from 12 to 20 m, a methane–nitrate transition zone (NMTZ) was observed, where δ13C values of methane and δ15N and δ18O of dissolved nitrate markedly increased in concert with decreasing concentrations of methane and nitrate. These data patterns, together with the results of a simple 1-D diffusion model linked with a degradation term, show that the nonlinear methane concentration profile cannot be explained by diffusion and that microbial oxidation of methane coupled with denitrification under anaerobic conditions is the most parsimonious explanation for these data trends. In the methane zone at the bottom of the NMTZ (20 to 22 m) δ15N of ammonium increased by 4 ‰, while ammonium concentrations decreased. In addition, a strong 15N enrichment of dissolved nitrate was observed at a water depth of 20 m, suggesting that anammox is occurring together with denitrification. The conversion of nitrite to N2 and nitrate during anammox is associated with an inverse N isotope fractionation and may explain the observed increasing offset (Δδ15N) of 26 ‰ between δ15N values of dissolved nitrate and nitrite at a water depth of 20 m compared to the Δδ15Nnitrate-nitrite of 11 ‰ obtained in the NMTZ at a water depth between 16 and 18 m. The associated methane concentration and stable-isotope profiles indicate that some of the denitrification may be coupled to AOM, an observation supported by an increased concentration of bacteria known to be involved in n-damo/denitrification with AOM (NC10 and Crenothrix) and anammox (“Candidatus Anammoximicrobium”) whose concentrations were highest in the methane and ammonium oxidation zones, respectively. This study shows the potential for a coupling of microbially mediated nitrate-dependent methane oxidation with anammox in stratified freshwater ecosystems, which may be important for affecting both methane emissions and nitrogen concentrations in lakes.Item Open Access Decadal Delays in Groundwater Recovery from Nitrate Contamination Caused by Low O2Reduction Rates(Wiley Periodicals, Inc. on behalf of the American Geophysical Union, 2018-11-13) Wild, Lisa M.; Mayer, Bernhard; Einsiedl, FlorianNitrate (NO urn:x-wiley:wrcr:media:wrcr23708:wrcr23708-math-0001) is one of the main pollutants in agriculturally impacted groundwater systems. The availability and reactivity of electron donors control the prevalent redox conditions in aquifers and past nitrate contamination of groundwater can be ameliorated if denitrification occurs. Using aqueous geochemistry data and the stable isotope composition of dissolved nitrate (δ15N and δ18O), we found that nitrate concentrations above the World Health Organization drinking water guideline were caused predominantly by manure and to a lesser extent by synthetic fertilizer applications and that denitrification was not a significant nitrate removal process in an aquifer in southern Germany underlying agricultural land with intensive hog farming. We also applied environmental isotopes (δ2H and δ18O, 3H/3He, and 14C) linked with a lumped parameter approach to determine apparent mean transit times (MTT) of groundwater that ranged from <5 years to >100 years. Furthermore, we determined low reduction rates of dissolved oxygen (O2) of 0.015 1/year for first-order kinetics. By extrapolating the O2 reduction rates beyond the apparent MTT ranges of sampled groundwater, denitrification lag times (time prior to commencement of denitrification) of approximately 114 years were determined. This suggests that it will take many decades to significantly reduce nitrate concentrations in the porous aquifer via denitrification, even if future nitrate inputs were significantly reduced.