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.
Agriculture is the major contributor of nitrogen to ecosystems, both by organic and inorganic fertilizers. Percolation of nitrate to groundwater and further transport to surface waters is assumed to be one of the major pathways in the fate of this nitrogen. The quantification of groundwater and associated nitrate flux to streams is still challenging. In particular because we lack understanding of the spatial distribution and temporal variability of groundwater and associated NO3- fluxes. In this preliminary study we will focus on the identification and quantification of groundwater and associated nitrate fluxes by combining high resolution distributed fiber-optic temperature sensing (DTS) with in situ UV photometry (ProPS). DTS is a new technique that is capable to measure temperature over distances of km with a spatial resolution of ca1 m and an accuracy of 0.01 K. It has been applied successfully to identify and quantify sources of groundwater discharge to streams. ProPS is a submersible UV process photometer, which uses high precision spectral analyses to provide single substance concentrations, in our case NO3-, at minute intervals and a detection limit of less than 0.05 mg l-1 (ca.0.01 mg NO3--Nl-1). We will conduct field experiments using artificial point sources of lateral inflow to test DTS and ProPS based quantification approaches and estimate their uncertainty. The selected study area is the Schwingbach catchment in Hessen, Germany, which has a good monitoring infrastructure. Preliminary research on hydrological fluxes and field observations indicate that the catchment favors the intended study.
Dissolved organic matter (DOM) is one major source of subsoil organic matter (OM). P5 aims at quantifying the impact of DOM input, transport, and transformation to the OC storage in the subsoil environment. The central hypotheses of this proposal are that in matric soil the increasing 14C age of organic carbon (OC) with soil depth is due to a cascade effect, thus, leading to old OC in young subsoil, whereas within preferential flowpaths sorptive stabilization is weak, and young and bioa-vailable DOM is translocated to the subsoil at high quantities. These hypotheses will be tested by a combination of DOC flux measurements with the comparative analysis of the composition and the turnover of DOM and mineral-associated OM. The work programme utilizes a DOM monitoring at the Grinderwald subsoil observatory, supplemented by defined experiments under field and labora-tory conditions, and laboratory DOM leaching experiments on soils of regional variability. A central aspect of the experiments is the link of a 13C-leaf litter labelling experiment to the 14C age of DOM and OM. With that P5 contributes to the grand goal of the research unit and addresses the general hypotheses that subsoil OM largely consists of displaced and old OM from overlying horizons, the sorption capacity of DOM and the pool size of mineral-associated OM are controlled by interaction with minerals, and that preferential flowpaths represent 'hot spots' of high substrate availability.
Der asiatische Sommermonsun ist charakterisiert durch hohe Konvektion über Südasien, die mit der asiatischen Monsun-Antizyklone (AMA) zusammenhängt, der sich von der oberen Troposphäre bis in die untere Stratosphäre (UTLS) erstreckt. Diese Antizyclone ist das ausgeprägteste Zirkulationsmuster in diesen Höhen während des borealen Sommer. Es ist bekannt, dass der Export von Monsunluft quasi-isentropisch aus der AMA sowohl im Osten als auch im Westen, einen großen Einfluss auf die Zusammensetzung der außertropischen unteren Stratosphäre hat. Jedoch sind die relative Stärken der beiden Wege bisher unbekannt. Der Transport von Luftmassen aus der AMA in die nördliche außertropische UTLS wirkt sich entscheidend auf die Chemie der Stratosphäre und ihrenStrahlungshaushalt (z.B. durch Transport von H2O, Aerosol oder ozonschädigende Stoffe) aus. Im Rahmen dieses Projekts AirExam wird der quasi-isentropischer Luftmassenexport aus der AMA durch verschiedene Wegen und seine Auswirkungen auf Chemie und Strahlung der außertropische UTLS quantifiziert durch u.a. HALO-Flugzeugmessungen (insbesondere aus die für Sommer 2023 geplanten PHILEAS-Kampagne), Simulationen mit dem Chemischen Transportmodell CLaMS und Strahlungsberechnungen. Unser Projekt AirExam wird sich mit den folgenden offenen Schlüsselfragen befassen:1) Welchen relativen Beitrag leisten die beiden quasi-horizontalen Transportwege (nach Westen und Osten) aus dem asiatischen Monsun-Antizyklon zur Zusammensetzung der außertropischen unteren Stratosphäre?2) Wie groß ist die jährliche Variabilität des Transports aus der asiatischen Monsun-Antizyklone in die außertropische untere Stratosphäre und was sind die Hauptquellenregionen auf der Erde Oberfläche?3) Was ist die Auswirkung des Wasserdampftransports aus der asiatischen Monsun-Antizyklone zum H2O-Budget der außertropischen UTLS und seine Strahlungswirkung?In unserem Projekt werden wir HALO-Messungen (insbesondere H2O) mit globalen 3-dimensionalen CLaMS-Simulationen kombinieren, die von neuen hochaufgelösten ERA-5-Reanalyse des ECMWF angetrieben werden. CLaMS-Simulationen auf der Grundlage von ERA-5 sind ein neues Instrument zur zuverlässigen Beschreibung von Transportprozessen in der Region des asiatischen Monsuns und seiner globalen Auswirkungen. Die Strahlungswirkung des durch den asiatischen Monsun verursachten H2O-Anstiegs im Sommer und Herbst wird mit Hilfe des Strahlungs-Transfercodes Edwards und Slingo berechnet. H2O ist das wichtigste Treibhausgas, und die Befeuchtung der Stratosphäre ist eine wichtige Triebkraft des Klimawandels. Unser Projekt AirExam wird die Auswirkungen des verstärkten H2O-Transports in die untere Stratosphäre quantifizieren und kann daher dazu beitragen, die potenziellen Risiken des Luftmassentransports aus der asiatischen Monsunregion auf die globale Stratosphäre zu bewerten.
Boron (B) is an essential microelement for plants. Despite the use of modern fertilization methods, B deficiency still causes losses in agricultural plant production. Even though many positive effects of B on plant growth and physiology have been reported, a large majority of B functions and the regulatory mechanisms controlling the B nutritional status remain unknown. The main objective of this project is to elucidate how the greatly B deficiency-sensitive Brassica crop plants process and regulate their B status during vegetative and reproductive growth. In this context, the project aims at identifying the mode of action of B in mechanisms regulating the B status itself and uncovering those mechanisms contributing to B efficiency in different genotypes. Plant species subjected to investigation will be the agronomically important oilseed and vegetable plant Brassica napus (rapeseed) and its close relative the genetic and molecular model plant Arabidopsis thaliana. Questions addressed within the scope of this project should lead to a detailed understanding of mechanisms controlling B uptake and allocation from the level of the whole plant down to the cellular level. B transport routes and rates will be determined in sink- and source tissues and in developmental periods with a particularly high B demand. A special focus will be on the identification of B transport bottlenecks and the analysis of B deficiency-sensitive transport processes to and within the highly B-demanding reproductive organs. Recent studies in Arabidopsis suggest that Nodulin26-like Intrinsic Proteins (NIPs), which belong to the aquaporin channel protein family, are essential for plant B uptake and distribution. The systematic focus on the molecular and physiological characterization of B. napus NIPs will clarify their role in B transport and will identify novel NIP-associated mechanisms playing key roles in the B response network.To further resolve the mostly unknown impact of the B nutritional status on gene regulation and metabolism, a transcript and metabolite profile of B-sufficient and B-deficient rapeseed plants will be generated. Additionally, an Arabidopsis transcription factor knockout collection (greater 300 lines) will be screened for abnormalities in responses to the B nutritional status. This will identify yet unknown B-responsive genes (transcription factors and their targets) and gene products (enzymes or metabolite variations) playing key roles in signalling pathways and mechanisms regulating the B homeostasis. Boron (in form of boric acid) and arsenite (As) share in all likelihood the same NIP-mediated transport pathways. To assess the consequences of this dual transport pathway the so far unstudied impact of the plants B nutritional status on the accumulation and distribution of As will be investigated in B. napus. Moreover, the current dimension of the As contamination of Brassica-based food products, to which consumers are exposed to, will be analyzed. usw.
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 detritusphere is an excellent model to study microbial-physicochemical interactions during degradation of the herbicide MCPA. Whereas during the first phase of SPP 1315 we focused on bacterial and fungal abundance at the soil litter interface and carbon flow between different compartments, the second phase will be devoted to elucidating complex regulation mechanisms of MCPA degradation in the detritusphere: (1) At the cellular level, co-substrate availability and laccase abundance might be important regulators, (2) at the community level, bacteria harbouring different classes of tfdA genes might control degradation of MCPA and (3) at the microhabitat level, interaction between MCPA degraders and organo-mineral surfaces as well as transport processes might be important regulators. The concept of hierarchical regulation of MCPA degradation will be included into the modelling of small-scale microbial growth, MCPA transport and MCPA degradation near the soil-litter interface.
Shallow groundwater of the huge deltaic systems of Asia like the Red River Delta in Vietnam is often enriched in inorganic arsenic (As), threatening the health of millions of residents. The massive abstraction of groundwater in these areas locally causes an irreversible mixing of arsenic-free groundwater resources with arsenic-rich groundwater. Increased concentrations of competitive anions, especially phosphate (PO43-), decrease the immobilization capacity of the sediments. During transport, the mobility of dissolved As in local aquifers is strongly influenced by adsorption to sedimentary and ubiquitously occurring iron(oxyhydr)oxides. Additionally, arsenic-rich groundwater is often enriched in reduced iron (Fe2+) as well, which is capable to react with iron(oxyhydr)oxides, thereby inducing mineral transformations. Such transformations permanently affect the arsenic adsorption and immobilization capacity of the sediments.Within the scope of this research project, the underlying mechanisms related to As transport and the resulting threat to arsenic-free groundwater resources will be characterized in cooperation with the Swiss Federal Institute of Aquatic Science and Technology (Eawag). The research concept aims at assessing the complex interactions within the arsenic-iron-phosphate-system under field conditions at a study site next to the Red River. First, filtration experiments using local groundwater enriched in As and PO43- will be used to determine the As adsorption capacity of different and previously geochemically characterized iron(oxyhydr)oxides. In a second step, sample carrier containing As loaded iron(oxyhydr)oxides will be introduced into surface near aquifer parts of the study site (via existing groundwater monitoring wells). These samples will be exposed to local groundwater characterized by increased As, Fe2+ and PO43- concentrations for the following nine months. Using the in situ exposition of predefined iron(oxyhydr)oxides, it will be possible to distinguish potential mineral transformations and their influences on the As immobilization capacity of the respective iron(oxyhydr)oxides. By combining the results and outcomes of the field experiments, new and important conclusions regarding the mobility of As can be drawn. The data can be used to create a hydrochemical transport model describing reactive As transport within the investigation area. In addition, the results of the in situ exposition experiments will allow to draw conclusions in respective to the long term As immobilization capacity of different iron(oxyhydr)oxides, which is an essential information regarding in situ decontamination techniques.
Groundwater contamination by organic compounds represents a widespread environmental problem. The heterogeneity of geological formations and the complexity of physical and biogeochemical subsurface processes, often hamper a quantitative characterization of contaminated aquifers. Compound specific stable isotope analysis (CSIA) has emerged as a novel approach to investigate contaminant transformation and to relate contaminant sources to downgradient contamination. This method generally assumes that only (bio)chemical transformations are associated with isotope effects. However, recent studies have revealed isotope fractionation of organic contaminants by physical processes, therefore pointing to the need of further research to determine the influence of both transport and reactive processes on the observed overall isotope fractionation. While the effect of gasphase diffusion on isotope ratios has been studied in detail, possible effects of aqueous phase diffusion and dispersion have received little attention so far.The goals of this study are to quantify carbon (13C/12C) and, for chlorinated compounds, chlorine (37Cl/35Cl) isotope fractionation during diffusive/dispersive transport of organic contaminants in groundwater and to determine its consequences for source allocation and assessment of reactive processes using isotopes. The proposed research is based on the combination of high-resolution experimental studies, both at the laboratory (i.e. zero-, one- and two-dimensional systems) and at the field scales, and solute transport modeling. The project combines the expertise in the field of contaminant transport with the expertise on isotope methods in contaminant hydrogeology.
Aktuelle wissenschaftliche Studien legen nahe, dass die aktuelle Erderwärmung durch Treibhausgasemissionen hervorgerufen wird, die vom Menschen verursacht sind. Um gegen diese Entwicklung geeignete Maßnahmen ergreifen zu können bzw. um zu überprüfen, ob solche Maßnahmen von Erfolg gekrönt sind, ist es notwendig, die Schadstoffkonzentrationen inklusive der zugehörigen Emissionsquellen genau zu kennen. Diese Informationen sind bisher jedoch sehr lückenhaft und beruhen auf sogenannten 'bottom-up' Berechnungen. Da diese Kalkulationen nicht auf direkten Messungen beruhen, weisen sie große Ungenauigkeiten auf und sind außerdem nicht in der Lage, bisher unbekannte Emissionsquellen zu identifizieren. In dem hier vorgestellten Projekt soll ein mesoskaliges Netzwerk für die Überwachung von Luftschadstoffen wie CO2, CH4, CO, NO2 und O3 aufgebaut werden, das auf dem neuartigen Konzept der differentiellen Säulenmessung beruht. Bei diesem Ansatz wird die Differenz zwischen den Luftsäulen luv- und leewärts einer Stadt gebildet. Diese Differenz ist proportional zu den emittierten Schadstoffen und somit eine Maßzahl für die Emissionen, welche in der Stadt generiert werden.Mithilfe dieser Methode wird es in Zukunft möglich sein, städtische Emissionen über lange Zeiträume hinweg zu überwachen. Damit können neue Informationen über die Generierung und Umverteilung von Luftschadstoffen gewonnen werden. Wir werden u.a. folgende zentrale Fragen beantworten: Wie verhält sich der tatsächliche Trend der CO2, CH4 und NO2 Emissionen in München über mehrere Jahre? Wo sind die Emissions-Hotspots? Wie akkurat sind die bisherigen 'bottom-up' Abschätzungen? Wie effektiv sind die Maßnahmen zur Emissionsreduzierung tatsächlich? Sind vor allem für Methan weitere Maßnahmen zur Reduzierung der Emissionen notwendig? Zu diesem Zweck werden wir ein vollautomatisiertes Messnetzwerk aufbauen und passende Methoden zur Modellierung entwickeln, welche u.a. auf STILT (Stochastic Time-Inverted Lagrangian Transport) und CFD (Computational Fluid Dynamics) basieren. Mithilfe der Modellierungsresultate werden wir eine Strategie entwerfen, wie städtische Netzwerke zur Überwachung von Luftschadstoffen aufgebaut werden müssen, um repräsentative Ergebnisse zu erhalten. Außerdem können mit den so gewonnenen städtischen Emissionszahlen z.B. dem Stadtreferat, den Stadtwerken München oder der Bayerischen Staatsregierung Möglichkeiten zur Beurteilung der Effektivität der angewandten Klimaschutzmaßnahmen an die Hand gegeben werden. Das hier vorgestellte Messnetzwerk dient somit als Prototyp, um die grundlegenden Fragen zum Aufbau eines solchen Sensornetzwerks zu klären, damit objektive Aussagen zu städtischen Emissionen möglich werden. Dieses Projekt ist weltweit einmalig und wird zukunftsweisende Ergebnisse liefern.
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