Summertime elemental mercury exchange of temperate grasslands on an ecosystem-scale

In order to estimate the air-surface mercury exchange of grasslands in temperate climate regions, fluxes of gaseous elemental mercury (GEM) were measured at two sites in Switzerland and one in Austria during summer 2006. Two classic micrometeorological methods (aerodynamic and modified Bowen ratio) have been applied to estimate net GEM exchange rates and to determine the response of the GEM flux to changes in environmental conditions (e. g. heavy rain, summer ozone) on an ecosystem-scale. Both methods proved to be appropriate to estimate fluxes on time scales of a few hours and longer. Average dry deposition rates up to 4.3 ng m(-2) h(-1) and mean deposition velocities up to 0.10 cm s(-1) were measured, which indicates that during the active vegetation period temperate grasslands are a small net sink for atmospheric mercury. With increasing ozone concentrations depletion of GEM was observed, but could not be quantified from the flux signal. Night-time deposition fluxes of GEM were measured and seem to be the result of mercury co-deposition with condensing water. Effects of grass cuts could also be observed, but were of minor magnitude

Influence of temperature and high acetate concentrations on methanogenensis in lake sediment slurries

Methanogenesis from main methane precursors H2/CO2 and acetate was investigated in a temperature range of 2-70 °C using sediments from Lake Baldegg, Switzerland. Psychrophilic, psychrotrophic, mesophilic, and thermophilic methanogenic microbial communities were enriched by incubations for 1-3 months of nonamended sediment slurries at 5, 15, 30, and 50 °C. Isotope experiments with slurries amended with 14C-labeled bicarbonate and 14C-2-acetate showed that in the psychrophilic community (enriched at 5 °C), about 95% of methane originated from acetate, in contrast to the thermophilic community (50 °C) where up to 98% of methane was formed from bicarbonate. In the mesophilic community (30 °C), acetate was the precursor of about 80% of the methane produced. When the hydrogen-carbon dioxide mixture (H2/CO2) was used as a substrate, it was directly converted to methane under thermophilic conditions (70 and 50 °C). Under mesophilic conditions (30 °C), both pathways, hydrogenotrophic and acetoclastic, were observed. At low temperatures (5 and 15 °C), H2/CO2 was converted into methane by a two-step process; first acetate was formed, followed by methane production from acetate. When slurries were incubated at high partial pressures of H2/CO2, the high concentrations of acetate produced of more than 20 mM inhibited acetoclastic methanogenesis at a temperature below 15 °C. However, slow adaptation of the psychrophilic microbial community to high acetate concentrations was observe

Ammonia Emissions from Swiss Agriculture and their Effects on Atmospheric Chemistry and Ecosystems

Ammonia (NH3) is an important atmospheric pollutant due to its contribution to secondary inorganic aerosol formation and its deposition and impacts on (semi-)natural ecosystems. Therefore various efforts have been made to limit emissions to the atmosphere. The predominant emission source in Switzerland is livestock agriculture, wherein NH3 is volatilised from ammonium contained in animal manure. While modelled NH3 emissions based on agricultural activity data indicate a minor decrease since 2000, concentration measurements do not reflect this trend. This can at least partly be attributed to a decline in the transformation of NH3 to particulate ammonium due to significantly decreased emission of oxidised nitrogen and sulfur compounds in the past decade. The partitioning between the gaseous and the particulate phase also determines the deposition pathway (dry or wet deposition) and thus the average lifetime and transport distance in the atmosphere. Gaseous NH3 is subject to fast dry deposition and is deposited preferentially to ecosystems close to the source. Once deposited into an ecosystem, NH3 leads to eutrophication and acidification of water and soils, which change the plant community composition and microbial functioning, especially in N-sensitive ecosystems. Although NH3 can also cause direct toxicity to plants, assessments of ecosystem impacts are generally collated using the critical load approach, which includes the input of all N compounds. These reveal that in 2020, 87% of forests, 94% of raised bogs, 74% of fens, and 42% of dry mountain grasslands likely experienced adverse impacts from N exceedances in Switzerland. To improve this situation, considerable NH3 emission abatement efforts are needed in the future

Correcting high-frequency losses of reactive nitrogen flux measurements

Flux measurements of reactive nitrogen compounds are of increasing importance to assess the impact of unintended emissions on sensitive ecosystems and to evaluate the efficiency of mitigation strategies. Therefore, it is necessary to determine the exchange of reactive nitrogen gases with the highest possible accuracy. This study gives insight into the performance of flux correction methods and their usability for reactive nitrogen gases. The eddy-covariance (EC) technique is today widely used in experimental field studies to measure land surface–atmosphere exchange of a variety of trace gases. In recent years, applying the EC technique to reactive nitrogen compounds has become more important since atmospheric nitrogen deposition influences the productivity and biodiversity of (semi)natural ecosystems and their carbon dioxide (CO2) exchange. Fluxes, which are calculated by EC, have to be corrected for setup-specific effects like attenuation in the high-frequency range. However, common methods for correcting such flux losses are mainly optimized for inert greenhouse gases like CO2 and methane or water vapor. In this study, we applied a selection of correction methods to measurements of total reactive nitrogen (6Nr) conducted in different ecosystems using the Total Reactive Atmospheric Nitrogen Converter (TRANC) coupled to a chemiluminescence detector (CLD). Average flux losses calculated by methods using measured cospectra and ogives were approximately 26 %–38% for a seminatural peatland and about 16 %–22% for a mixed forest. The investigation of the different methods showed that damping factors calculated with measured heat and gas flux cospectra using an empirical spectral transfer function were most reliable. Flux losses of 6Nr with this method were on the upper end of the median damping range, i.e., 38% for the peatland site and 22% for the forest site. Using modified Kaimal cospectra for damping estimation worked well for the forest site but underestimated damping for the peatland site by about 12 %. Correction factors of methods based on power spectra or on site-specific and instrumental parameters were mostly below 10 %. Power spectra of 6Nr were heavily affected – likely by white noise – and deviated substantially at lower frequencies from the respective temperature (power) spectra. Our study supports the use of an empirical method for estimating flux losses of 6Nr or any reactive nitrogen compound and the use of locally measured cospectra

Using the inverse dispersion method to determine methane emissions from biogas plants and wastewater treatment plants with complex source configurations

Wastewater treatment plants (WWTPs) and biogas plants (BGPs) are significant sources of methane (CH4), with a combined share of around 40 % within the waste sector of the Swiss national emission inventory. We conducted whole-plant CH4 emission measurements at two WWTPs and four agricultural BGPs in Switzerland using the inverse dispersion method (IDM). This involved open-path concentration measurements up- and downwind of the plant in combination with a backward Lagrangian stochastic (bLS) model. WWTPs in particular consist of multiple CH4 sources with different areas and emission strengths. For the combination of the individual emission sources in the bLS modelling, three different calculation approaches with different levels of detail were applied: (i) single source over enveloping polygon area, (ii) uniform emission density for all individual source areas, (iii) specified relative weighting of individual sources based on literature data. Average CH4 emissions for WWTP 1 and WWTP 2 were 0.82 kg h-1 and 0.61 kg h-1 and scaled to population equivalents (PE) 166 g PE-1 y-1 and 381 g PE-1 y-1, respectively. BGPs CH4 emissions varied between 0.39 kg h-1 and 2.22 kg h-1, corresponding to less than 5 % of the plants’ CH4 production. The highest numbers were due to measurements during other than normal operating conditions. The emissions of WWTPs and BGPs comply with literature values. Approach (iii) with source weighting led to a difference of up to 43 % for the two WWTPs compared to the assumption of uniform emissions. Furthermore, we demonstrate how multiple open-path concentration measurements can be combined and how the measurements can be corrected for nearby external CH4 sources not belonging to the investigated plants. The results of the present study contribute to improved emission data from the waste sector

Quantification of methane emissions from waste water treatment plants

Quantification of gaseous emissions from waste water treatment plants (WWTPs) is challenging due to the heterogeneity of the emissions in space and time. The inverse dispersion method (IDM) using concentration and turbulence measurements in combination with a backward Lagrangian stochastic (bLS) dispersion model based on Flesch et al. (2004) is a promising option. It is increasingly used to determine gaseous emissions from confined sources (Flesch et al., 2009; VanderZaag et al., 2014), as it offers high flexibility at reasonable costs. For the application on WWTPs the bLS model assumption of spatially homogeneous turbulence, which implies absence of obstacles as buildings and trees that disturbe the flow, is often not fulfilled. However, studies showed that with the correct instrument setup and data filtering the bLS can be used for emission estimates. Methane emissions from two WWTPs of different type and size were quantified using the IDM with the bLS model. Methane concentrations were analysed with open-path tunable diode laser spectrometers (GasFinder, Boreal Laser, Inc., Edmonton, Alberta, Canada) placed up- and downwind of the source. At each site at least 20 days of measurements averaged to 30-minutes intervals are available. Here we present first results from these two WWTPs emission estimates

Reducing N fertilization in the framework of the European Farm to Fork strategy under global change: Impacts on yields, N₂O emissions and N leaching of temperate grasslands in the Alpine region

Context The reduction of N fertilization in agriculture as part of the Farm to Fork (F2F) strategy plays a central role in the integrated nutrient management action plan of the European Commission. However, the implications of this strategy for mitigating N losses and possible side-effects on grassland yields under global change are largely unknow. Objective We examined how a 20% reduction in N fertilization according to the F2F strategy is likely to impact yields, N2O emissions and N leaching of four intensively managed temperate grasslands in the Alpine region, two of them located in Switzerland, the other two in Germany. Methods Following automatic data-driven calibration supported by inverse modeling and a cross-validation step, the process-based model DayCent was used for conducting the analysis. Global change scenarios under the representative concentration pathways (RCPs) 4.5 and 8.5 and a baseline scenario (current climate) were created for the time frame 2041–2060 with the help of the stochastic weather generator LARS-WG. Results and conclusions Our results indicated that, under current conditions of climate and CO2 levels (400 ppm), a 20% decrease in N fertilization would lead to a 5% drop in yields, but also in a 15% decline in N2O emissions and a 21% decline in N leaching (largely as NO3−). Under global change conditions (i.e., climate change and higher atmospheric CO2 levels), we found that increased yields, mainly induced by higher CO2 levels, are likely to compensate for yield losses resulting from the reduction in N fertilization. In addition, we found that the effectiveness of the F2F strategy to mitigate N losses is likely to be preserved under global change, still with stronger effect on N leaching. The F2F-induced decline in N losses was stronger when the latter were expressed per unit of harvested dry matter, i.e., up to 17% for N2O and up to 42% for N leaching. Although significant, these abatements in N losses are still below the 50% reduction level envisaged by the F2F strategy. Actions related to other axes of the strategy (e.g., sustainable food consumption) will be necessary to further reduce N fertilization and, therefore, to reach this ambitious goal. Significance Our results highlight the usefulness of models in accounting for interacting effects of global change and mitigation practices on multiple ecosystem services of grasslands. They allow quantification of the impact of new policies

Reactive nitrogen fluxes over peatland and forest ecosystems using micrometeorological measurement techniques

Interactions of reactive nitrogen (Nr) compounds between the atmosphere and the earth's surface play a key role in atmospheric chemistry and in understanding nutrient cycling of terrestrial ecosystems. While continuous observations of inert greenhouse gases through micrometeorological flux measurements have become a common procedure, information about temporal dynamics and longer-term budgets of Nr compounds is still extremely limited. Within the framework of the research projects NITROSPHERE and FORESTFLUX, field campaigns were carried out to investigate the biosphere–atmosphere exchange of selected Nr compounds over different land surfaces. The aim of the campaigns was to test and establish novel measurement techniques in eddy-covariance setups for continuous determination of surface fluxes of ammonia (NH3) and total reactive nitrogen (ΣNr) using two different analytical devices. While high-frequency measurements of NH3 were conducted with a quantum cascade laser (QCL) absorption spectrometer, a custom-built converter called Total Reactive Atmospheric Nitrogen Converter (TRANC) connected and operated upstream of a chemiluminescence detector (CLD) was used for the measurement of ΣNr. As high-resolution data of Nr surface–atmosphere exchange are still scarce but highly desired for testing and validating local inferential and larger-scale models, we provide access to campaign data including concentrations, fluxes, and ancillary measurements of meteorological parameters. Campaigns (n=4) were carried out in natural (forest) and semi-natural (peatland) ecosystem types. The published datasets stress the importance of recent advancements in laser spectrometry and help improve our understanding of the temporal variability of surface–atmosphere exchange in different ecosystems, thereby providing validation opportunities for inferential models simulating the exchange of reactive nitrogen. The dataset has been placed in the Zenodo repository (https://doi.org/10.5281/zenodo.4513854; Brümmer et al., 2022) and contains individual data files for each campaign

Assessment of the inverse dispersion method for the determination of methane emissions from a dairy housing

Methane (CH4) emissions from dairy housings, mainly originating from enteric fermentation of ruminating animals, are a significant source of greenhouse gases. The quantification of emissions from naturally ventilated dairy housings is challenging due to the spatial distribution of sources (animals, housing areas) and variable air exchange. The inverse dispersion method (IDM) is a promising option, which is increasingly used to determine gaseous emissions from stationary sources, as it offers high flexibility in the application at reasonable costs. We used a backward Lagrangian stochastic model combined with concentration measurements by open-path tunable diode laser spectrometers placed up- and downwind of a naturally ventilated housing with 40 dairy cows to determine the CH4 emissions. The average emissions per livestock unit (LU) were 317 (±44) g LU−1 d−1 and 267 (±43) g LU−1 d−1 for the first and second campaign, in September – October and November – December, respectively. For each campaign, inhouse tracer ratio measurements (iTRM) were conducted in parallel during two subperiods. For simultaneous measurements, IDM showed average emissions which were lower by 8% and 1% than that of iTRM, respectively, for the two campaigns. The differences are within the uncertainty range of any of the two methods. The IDM CH4 emissions were further analysed by wind direction and atmospheric stability and no differences in emissions were found. Overall, IDM showed its aptitude to accurately determine CH4 emissions from dairy housings or other stationary sources if the site allows adequate placement of sensors up- and downwind in the prevailing wind direction. To acquire reliable emission data, depending on the data loss during measurements due to quality filtering or instrument failure, a measuring time of at least 10 days is required

Influence of temperature and high acetate concentrations on methanogenensis in lake sediment slurries

Methanogenesis from main methane precursors H2/CO2 and acetate was investigated in a temperature range of 2–70 °C using sediments from Lake Baldegg, Switzerland. Psychrophilic, psychrotrophic, mesophilic, and thermophilic methanogenic microbial communities were enriched by incubations for 1–3 months of nonamended sediment slurries at 5, 15, 30, and 50 °C. Isotope experiments with slurries amended with 14C-labeled bicarbonate and 14C-2-acetate showed that in the psychrophilic community (enriched at 5 °C), about 95% of methane originated from acetate, in contrast to the thermophilic community (50 °C) where up to 98% of methane was formed from bicarbonate. In the mesophilic community (30 °C), acetate was the precursor of about 80% of the methane produced. When the hydrogen–carbon dioxide mixture (H2/CO2) was used as a substrate, it was directly converted to methane under thermophilic conditions (70 and 50 °C). Under mesophilic conditions (30 °C), both pathways, hydrogenotrophic and acetoclastic, were observed. At low temperatures (5 and 15 °C), H2/CO2 was converted into methane by a two-step process; first acetate was formed, followed by methane production from acetate. When slurries were incubated at high partial pressures of H2/CO2, the high concentrations of acetate produced of more than 20 mM inhibited acetoclastic methanogenesis at a temperature below 15 °C. However, slow adaptation of the psychrophilic microbial community to high acetate concentrations was observed