Chromium (Cr) is introduced into the environment by several anthropogenic activities. A striking ex-ample is the area around Kanpur in the Indian state of Uttar Pradesh, where large amounts of Cr-containing wastes have been recently illegally deposited. Hexavalent Cr, a highly toxic and mobile contaminant, is present in significant amounts in these wastes, severely affecting the quality of sur-roundings soils, sediments, and ground waters. The first major goal of this study is to clarify the solid phase speciation of Cr in these wastes and to examine its leaching behavior. X-ray diffraction and synchrotron-based X-ray absorption spectroscopy techniques will be employed for quantitative solid phase speciation of Cr. Its leaching behavior will be studied in column experiments performed at un-saturated moisture conditions with flow interruptions simulating monsoon rain events. Combined with geochemical modeling, the results will allow the evaluation of the leaching potential and release kinetics of Cr from the waste materials. The second major goal is to investigate the spatial distribution, speciation, and solubility of Cr in the rooting zone of chromate-contaminated soils surrounding the landfills, and to study the suitability of biochar as novel soil amendment for mitigating the deleterious effects of chromate pollution. Detailed field samplings and laboratory soil incubation studies will be carried out with two agricultural soils and biochar from the Kanpur region.
In this project we experimentally explore the transport of engineered inorganic nanoparticles (EINP) through soils. This is done for original EINPs and some pre-aged form. Transport of NPs in soil is expected to be different from that of reactive solutes, in that hydrodynamic drag, inertial and shear forces as well as the affinity to water-gas interfaces are expected to be more relevant. Hence, the mobility of EINPs in soil is highly sensitive to the morphology of the porous structure and the dynamics of water saturation.This project provides the pore network structure for natural soils using X-ray micro-tomography to allow for an up-scaling of pore-scale interactions explored by project partners to the scale of soil horizons. The pore structure is represented by a network model suitable for pore scale simulations including the dynamics of water-gas interfaces.Pore network simulations will be compared to column experiments for conservative tracers as well as for unaltered and pre-aged EINPs (obtained from INTERFACE). This includes steady state flow scenarios for saturated (ponding) and unsaturated conditions as well as for transient flow to explore the impact of moving water-gas interfaces. The final goal is to arrive at a consistent interpretation of experimental findings and numerical simulations to develop a module for modelling EINP transfer through soil as a function of particle properties, soil structural characteristics and external forcing in terms of flux boundary conditions.
The relevance of biogeochemical gradients for turnover of organic matter and contaminants is yet poorly understood. This study aims at the identification and quantification of the interaction of different redox processes along gradients. The interaction of iron-, and sulfate reduction and methanogenesis will be studied in controlled batch and column experiments. Factors constraining the accessibility and the energy yield from the use of these electron acceptors will be evaluated, such as passivation of iron oxides, re-oxidation of hydrogen sulfide on iron oxides. The impact of these constraints on the competitiveness of the particular process will then be described. Special focus will be put on the evolution of methanogenic conditions in systems formerly characterized by iron and sulfate reducing condition. As methanogenic conditions mostly evolve from micro-niches, methods to study the existence, evolution and stability of such micro-niches will be established. To this end, a combination of Gibbs free energy calculations, isotope fractionation and tracer measurements, and mass balances of metabolic intermediates (small pool sizes) and end products (large pool sizes) will be used. Measurements of these parameters on different scales using microelectrodes (mm scale), micro sampling devices for solutes and gases (cm scale) and mass flow balancing (column/reactor scale) will be compared to characterize unit volumes for organic matter degradation pathways and electron flow. Of particular interest will be the impact of redox active humic substances on the competitiveness of involved terminal electron accepting processes, either acting as electron shuttles or directly providing electron accepting capacity. This will be studied using fluorescence spectroscopy and parallel factor analysis (PARAFAC) of the gained spectra. We expect that the results will provide a basis for improving reactive transport models of anaerobic processes in aquifers and sediments.
Nitrogen isotope ratios can provide important constraints on natural N cycles. In order to use natural abundance stable isotope ratios of dissolved inorganic N species as a means to trace fluxes and transformations of N in aquatic systems, however, it is imperative to understand the isotope effects associated with these specific N transformations. This will also provide information on the transformations themselves. Yet, the possible impact of N2 production processes other than denitrification on global and regional N-isotope budgets has been ignored thus far. Lake Lugano is an excellent model biosystem for an anthropogenically impacted lake. Previous studies have revealed that this lake represents an important sink for fixed N. In addition, they indicate the presence of suboxic consumption of ammonium and, thus, suggest that 'non-traditional' N2 production processes (e.g., anammox) are active in anaerobic portions of the lake. This project addresses the following main research questions: What are the different metabolic pathways of suboxic N2 production in the Lake Lugano water column and in sediments? What are the associated N-isotope effects? What are the respective transformation rates and fluxes? Which microorganisms are responsible for observed N transformations? Combining hydrochemical, microbiological (phylogenetic/molecular genetic analyses, measurements of enzyme activities), with organic-geochemical (anammox lipid analysis) and isotopic techniques (natural abundance of nitrate, ammonium, nitrous oxide isotope ratios, as well as 15N tracer experiments), the project attempts to gain complementary information on specific N transformations and mechanisms of N2 loss in the Lake Lugano water column and sediments, on the microorganisms involved in these transformations, their relevance for the Lake Lugano nitrogen
Bioavailable nitrogen (N) from anthropogenic sources is an important driver of lacustrine eutrophication. However, N loading in lakes is partially mitigated by microbially mediated processes that take place in redox transition zones (RTZ) within the water column and in sediments. RTZ are also sites of methane (CH4) and nitrous oxide (N2O) production and consumption. As a result of anthropogenic activities, emissions of these greenhouse gases to the atmosphere have significantly increased over the past decades. Lake Lugano is an excellent model system for an anthropogenically impacted lake that represents a hot-spot of quantitative redox-driven transformations involving the green house gases CH4 and N2O, as well as other N species acting as important macro nutrients. Previous studies have revealed that this lake represents an important sink for fixed N and that the anoxic deep-waters and sediments contain high concentrations of CH4. Through the application of stable isotopic, molecular ecological and geochemical techniques, laboratory cultivation and (radio-) tracer studies, the project will try (i) to understand the metabolic pathway involved in N and CH4 elimination in Lake Lugano, (ii) to assess the metabolic rates, at which the respective elimination processes take place, as well as their variability in time and space, (iii) to constrain the isotope effects associated with specific N and CH4 transformations, and (iv) to provide information about the microorganisms involved in these transformations. Thereby, a particularly focus is put on reactions that have essentially been neglected in lacustrine studies thus far, namely the anarobic oxidation of ammonium (anammox) and the anaerobic oxidation of methane (AOM). The project will provide the first comprehensive characterization of early diagenetic reactions in Lake Lugano. Moreover, it may allow insights into novel modes of autotrophic life in lakes. Finally, quantitative estimates of N and CH4 elimination in both the water column and sedimentary RTZ of Lake Lugano will be a prerequisite for ecosystem-scale N and C budgets. Thus, the project will provide important information that is directly pertinent to the health of Lake Lugano in particular, and eutrophied south alpine lakes in general.
Two related SNF-projects are the Swiss contribution to the Lake Van Drilling Project being carried out by the International Continental Scientific Drilling Program (ICDP). This Lake Van Drilling project (PALEOVAN) the key to trigger the newly established SNF-supported Swiss membership in ICDP. One proposal covers the Swiss share of the drilling operations to recover several hundred meters of sediments. The other proposal addresses the scientific activities of the involved Swiss research groups. Lake Van (eastern Anatolia, Turkey), the fourth largest terminal lake on Earth, is surrounded by lively volcanoes within a tectonically active area. Lake Van's annually-laminated sediments are expected to be excellent paleoclimate and paleoenvironment archive because they contain a long and continuous continental sequence that covers several glacial-interglacial cycles (ca.500 kyr). Therefore, ICDP identified Lake Van is a key site to investigate climatic, environmental, volcanic and tectonic evolution during the last few hundred thousands years of the Near East in the cradle of human civilization. This Swiss initiative embedded in the overarching ICDP Drilling project on Lake Van consist of five complementary research modules: Module A: Sedimentology and stratigraphic framework and implications for lake level changes and paleoseismology. Module B: Geochemical analyses of solid phase (climate proxies) and fluid phase. Module C: Organic geochemistry, biomarkers, 14C dating of single compounds. Module D: 10Be as a tracer of solar and geomagnetic variability and erosion rate. 10Be as well as 14C and 36Cl provide a unique tool to reconstruct the history of solar variability and changes in the geomagnetic field intensity. The large laminated sediment body of Lake Van allows to study the evolution of long-lived radio nuclides at high temporal resolution on much longer time scales than those being assessable by ice-cores. Module E: Noble gases as proxy for vertical fluid transport in the sediment column and lake level fluctuation.
Sulfur isotope fractionation (34S/32S) has been used since the late 1940s to study the chemical and biological sulfur cycle. While large isotope fractionations during bacterial sulfate reduction were used successfully to interpret, e.g., accumulation of sulfate in ancient oceans or the evolution of early life, much less is known about fractionation during sulfide oxidation. The fractionation between the two end-members sulfide and sulfate is commonly much smaller and inconsistencies exist whether substrate or product are enriched. These inconsistencies are explained by a lack of knowledge on oxidation pathways and rates as well as intermediate sulfur species, such as elemental sulfur, polysulfides, thiosulfate, sulfite, or metalloid-sulfide complexes (e.g. thioarsenates), potentially acting as 34S sinks.In the proposed project, we will develop a method for sulfur species-selective isotope analysis based on separation by preparative chromatography. Separation of Sn2- and S0 will be achieved after derivatization with methyl triflate on a C18 column, separation of the other sulfur species in an alkaline eluent on an AS16 column. Sulfur in the collected fractions will be extracted directly with activated copper chips (Sn2-, S0), or precipitated as ZnS (S2-) or BaSO4 and analyzed by routine methods as SO2. Results of this species-selective approach will be compared to those from previous techniques of end-member pool determinations and sequential precipitations.The method will be applied to sulfide oxidation profiles at neutral to alkaline hot springs at Yellowstone National Park, USA, where we detected intermediate sulfur species as important species. Determining 34S/32S only in sulfide and sulfate, our previous study has shown different fractionation patterns for two hot spring drainages with sulfide oxidation profiles that seemed similar from a geochemical perspective. The reasons for the different isotopic trends are unclear. In the present project, we will differentiate species-selective abiotic versus biotic fractionation using on-site incubation experiments with the chemolithotrophic sulfur-oxidizing bacteria Thermocrinis ruber as model organism. For selected samples, we will test whether 33S and 36S further elucidate species-selective sulfide oxidation patterns. We expect that lower source sulfide concentrations increase elemental sulfur disproportionation, thus increase redox cycling and isotope fractionation. We also expect that the larger the concentration of intermediate sulfur species, including thioarsenates, the larger the isotope fractionation. Following fractionation in species-selective pools, we will be able to clarify previously reported inconsistencies of 34S enrichment in substrate or product, elucidate sulfide oxidation pathways and rates, and reveal details about sulfur metabolism. Our new methodology and field-based data will be a basis for more consistent studies on sulfide oxidation in the future.
The aim of the project is to investigate the role of physical forcing, resource availability, and organismic interactions for the spatial and temporal distribution patterns of plankton in lakes. The research is focused on the distribution patterns of the buoyant cyano bacterium Planklothrix rubescens in Lake Ammer and compares the abundance of P. rubescens with the temporal and spatial variability of abiotic conditions and of phyto- and zooplankton. The main hypotheses are that (1) transport by internal wave motions has a substantial influence on the horizontal distribution patterns of P. rubescens and also affects the distribution of other phyto- and zooplankton; (2) vertical water column motions associated with internal waves cause fluctuations in the vertical layering of P. rubescens and thus alters its competitive abilities; (3) horizontal differences in habitat conditions, i.e. limited vertical water column depth in bays and resource gradients near river inflows, result in longer-term characteristic horizontal distribution patterns of P. rubescens and other plankton; (4) layers of toxic P. rubescens may interfere with the vertical migration of zooplankton. These research questions will be addressed in extensive field experiments measuring horizontal and vertical distribution patterns of plankton and abiotic conditions at temporal scales ranging from minutes to several weeks. In-situ measuring techniques for plankton and abiotic parameters, providing sufficient teniporal and spatial resolution, will be combined with water sample analyses to support them. The distribution of P. rubescens will be measured by using our newly developed in-situ technique that combines information from optic and acoustic instruments. The field experiments will be complemented with 3D and 1D model approaches. The intension of the modeling work is to support the interpretation of the field data by performing numerical experiments that investigate the response of horizontal distribution patterns of P. rubescens to physical forcing, patchy nutrient distribution (e.g. river inflow) or the presence of a shallow bay and by studying the implications of water column depth, internal wave induced fluctuations in light intensity, and grazing for the layering of p. rubescens in a vertical water column.
The major goal of this new subproject is to estimate transport and fluxes of solutes between the bottom boundary layer, the stratified interior ocean and the ocean mixed layer on the continental slope and shelf regions of the Peruvian and Mauritanian Oxygen Minimum Zones (OMZ). The objectives will be achieved by estimating diapycnal and advective fluxes using two different methodological approaches: The first is basedon the measurement of the radium isotope distribution in sediments and in the water column. The second approach will use a combination of oceanographic measuring systems for the determination of turbulences, currents and hydrography. Subproject A8 will contribute to the understanding of the solute budget of the OMZ's and establishes a link between the benthic and pelagic research foci within the SFB 754.
Mercury (Hg) is a persistent micropollutant presenting a substantial risk to the environment and an important threat to the human health. Past and present Hg contaminations of surface waters are thus of major concern due to the potential of Hg to accumulate in biota and magnify in the food chain. Therefore, the improved understanding of the relationship between Hg dispersion, distribution among sediments, particles, colloids and dissolved fractions, as well as accumulation and impact to biota is a prerequisite to fully assess the Hg threat to the aquatic systems and human health. By applying an integrated approach including a combination of field studies, laboratory analyses and numerical simulations, the present proposal aims to assess the impact of the Hg in the industrially impacted surface water bodies in Romania and to identify the possible threat on these resources The project focuses on River Olt basin, as one of the most impacted surface water body in Romania, altered by the cascade dam construction and under extensive past and present industrial activity. The Rm Valcea region comprises a high number of industrial companies including a large chlor-alkali plant (Oltchim), which is recognized as important point sources of Hg. A large array of hydro(geo)logical, physical, chemical, and ecotoxicological tools will be used to address the following key issues: - Performance of Hg survey and estimation the pollution extent in water and sediments; - Determination of the transport and dispersion of Hg in water column and sediments; - Improvement of the understanding on the behaviour of Hg associated to colloids, inorganic particles and organic matter; - Assessment of the bioaccumulation and effect of Hg to different organisms with emphasis on the primary producers in particular microalgae and macrophytes; - Evaluation of the food chain transfer and possible risks for the human health. The project will largely contribute to the understanding of mercury fate and impact in the contaminated systems and improved knowledge on complex processes governing the transfer and impact of Hg from the contaminated surface waters to humans. The project is also expected to contribute broadly to solving societal problems in Romania and to provide a scientific base for a sound definition of the existing problem and understand the causal chain, as well as it will help to develop efficient and cost-effective measures for protection. Strengthening the capacity, improving integration of scientists in the international network as well as developing 'best practices' for impact assessment of pollutants are other major outcomes of the project. They will be a significant step forward contaminant assessment in the entire Danube - Black Sea - Caspian Sea region, as it is a commonly accepted that historical industrial pollution from former communist times represents a significant threat for public health.
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