The broad objective of the research is to gain a fundamental understanding of the surface reaction chemistry of exhaust catalysts operating under cycling conditions. Using an integrated theoretical approach we specifically target NOx abatement, with particular emphasis on the appearance and destruction of surface oxide phases as the reactor conditions cycle from oxidative to reductive during the operation of the NOx Storage Reduction (NSR) catalyst system. Methodologically this requires material-specific, quantitative and explicitly time-dependent simulation tools that can follow the evolution of the system over the macroscopic time-scales of NSR cycles, while simultaneously accounting for the atomic-scale site heterogeneity and spatial distributions at the evolving surface. To meet these challenging demands we will develop a novel multi-scale methodology relying on a multi-lattice first-principles kinetic Monte Carlo (kMC) approach. As representative example the simulations will be carried out on a PdO(101)/Pd(100) surface oxide model, but care will be taken to ensure a generalization of the multi-lattice first-principles kMC approach to other systems in which phase transformations may occur and result in a change in the surface lattice structure depending upon environmental variables.
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.
Recent and predicted increases in extremely dry and hot summers emphasise the need for silvicultural approaches to increase the drought tolerance of existing forests in the short-term, before adaptation through species changes may be possible. We aim to investigate whether resistance during droughts, as well as the recovery following drought events (resilience), can be increased by allocating more growing space to individual trees through thinning. Thinning increases access of promoted trees to soil stored water, as long as this is available. However, these trees may also be disadvantaged through a higher transpirational surface, or the increased neighbourhood competition by ground vegetation. To assess whether trees with different growing space differ in drought tolerance, tree discs and cores from thinning experiments of Pinus sylvestris and Pseudotsuga menziesii stands will be used to examine transpirational stress and growth reduction during previous droughts as well as their subsequent recovery. Dendroecology and stable isotopes of carbon and oxygen in tree-rings will be used to quantify how assimilation rate and stomatal conductance were altered through thinning. The results will provide crucial information for the development of short-term silvicultural adaptation strategies to adapt forest ecosystems to climate change. In addition, this study will improve our understanding of the relationship between resistance and resilience of trees in relation to extreme stress events.
Irrigation in the Yanqi Basin, Sinkiang, China has led to water table rise and soil salination. A model is used to assess management options. These include more irrigation with groundwater, water saving irrigation techniques and others. The model relies on input data from remote sensing.The Yanqi Basin is located in the north-western Chinese province of Xinjiang.This agriculturally highly productive region is heavily irrigated with water drawn from the Kaidu River. The Kaidu River itself is mainly fed by snow and glacier melt from the Tian Mountain surrounding the basin. A very poor drainage system and an overexploitation of surface water have lead to a series of environmental problems: 1. Seepage water under irrigated fields has raised the groundwater table during the last years, causing strongly increased groundwater evaporation. The salt dissolved in the groundwater accumulates at the soil surface as the groundwater evaporates. This soil salinization leads to degradation of vegetation as well as to a loss of arable farmland. 2. The runoff from the Bostan Lake to the downstream Corridor is limited since large amount of water is used for irrigation in the Yanqi Basin. Nowadays, the runoff is maintained by pumping water from the lake to the river. The environmental and ecological system is facing a serious threat.In order to improve the situation in the Yanqi Basin, a jointly funded cooperation has been set up by the Institute of Environmental Engineering, Swiss Federal Institute of Technology (ETH) , China Institute of Geological and Environmental Monitoring (CIGEM) and Xinjiang Agricultural University. The situation could in principle be improved by using groundwater for irrigation, thus lowering the groundwater table and saving unproductive evaporation. However, this is associated with higher cost as groundwater has to be pumped. The major decision variable to steer the system into a desirable state is thus the ratio of irrigation water pumped from the aquifer and irrigation water drawn from the river. The basis to evaluate the ideal ratio between river and groundwater - applied to irrigation - will be a groundwater model combined with models describing the processes of the unsaturated zone. The project will focus on the following aspects of research: (...)
Outbreaks of foodborne illness linked to consumptions of fresh, or partially processed, agricultural products are a growing concern in industrialized and developing countries. The incidence of human pathogens on fresh fruits and vegetables is often related to the use of recycled wastewaster in surface irrigation as well as high amounts of animal manure in agricultural management practice. Thereby the soil inhabiting fauna plays an important role in the transport and dissemination of microorganisms. The focus of the proposed project is on nematodes, well known vectors for bacteria and viruses in soil. The major goals are to: (1) survey human pathogens in soil and on/in free-living and plant parasitic nematodes in agriculture field sites irrigated with recycled wastewater or fertilized with fresh animal manure in Israel and the Palestinian Authority, (2) assess the function of nematodes as vectors in transmitting bacteria from microbial hot spots to plants, and (3) localize bacteria on and/or within the nematode and identify bacterial factors required for survival in the nematode host. Understanding the mechanisms involved in dissemination of human pathogens by nematodes will enhance the ability to develop practical means to minimize contamination of fresh produce and increase safety in food production.
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.
In structured soils, the interaction of percolating water and reactive solutes with the soil matrix is mostly restricted to the surfaces of preferential flow paths. Flow paths, i.e., macropores, are formed by worm burrows, decayed root channels, cracks, and inter-aggregate spaces. While biopores are covered by earthworm casts and mucilage or by root residues, aggregates and cracks are often coated by soil organic matter (SOM), oxides, and clay minerals especially in the clay illuviation horizons of Luvisols. The SOM as well as the clay mineral composition and concentration strongly determine the wettability and sorption capacity of the coatings and thus control water and solute movement as well as the mass exchange between the preferential flow paths and the soil matrix. The objective of this proposal is the quantitative description of the small-scale distribution of physicochemical properties of intact structural surfaces and flow path surfaces and of their distribution in the soil volume. Samples of Bt horizons of Luvisols from Loess will be compared with those from glacial till. At intact structural surfaces prepared from soil clods, the spatial distribution (mm-scale) of SOM and clay mineral composition will be characterized with DRIFT (Diffuse reflectance infrared Fourier transform) spectroscopy using a self-developed mapping technique. For samples manually separated from coated surfaces and biopore walls, the contents of organic carbon (Corg) and the cation exchange capacity (CEC) will be analyzed and related to the intensities of specific signals in DRIFT spectra using Partial Least Square Regression (PLSR) analysis. The signal intensities of the DRIFT mapping spectra will be used to quantify the spatial distribution of Corg and CEC at these structural surfaces. The DRIFT mapping data will also be used for qualitatively characterizing the small scale distribution of the recalcitrance, humification, and microbial activity of the SOM from structural surfaces. The clay mineral composition of defined surface regions will be characterized by combining DRIFT spectroscopic with X-ray diffractometric analysis of manually separated samples. Subsequently, the spatial distribution of the clay mineral composition at structural surfaces will be determined from the intensities of clay mineral-specific signals in the DRIFT mapping spectra and exemplarily compared to scanning electron microscopic and infrared microscopic analysis of thin sections and thin polished micro-sections. The three-dimensional spatial distribution of the total structural surfaces in the volume of the Bt horizons will be quantified using X-ray computed tomography (CT) analysis of soil cores. The active preferential flow paths will be visualized and quantified by field tracer experiments. These CT and tracer data will be used to transfer the properties of the structural surfaces characterized by DRIFT mapping onto the active preferential flow paths in the Bt horizons.
We consider clay minerals, iron oxides and charcoal as major components controlling the formation of interfaces relevant for sorption of organic chemicals, as they control the assemblage of organic matter and mineral particles. We studied the formation of interfaces in batch incubation experiments with inoculated artificial soils consisting of model compounds (clay minerals, iron oxide, char) and natural soil samples. Results show a relevant contribution of both iron oxides and clay minerals to the formation of organic matter as sorptive interfaces for hydrophobic compounds. Thus, we intend to focus our work in the second phase on the characterization of the interface as formed by organic matter associated with clay minerals and iron oxides. The interfaces will be characterized by the BET-N2 and ethylene glycol monoethyl ether (EGME) methods and 129Xe and 13C NMR spectroscopy for determination of specific surface area, sorptive domains in the organic matter and microporosity. A major step forward is expected by the analysis of the composition of the interface at different resolution by reflected-light microscopy (mm scale), SEM (scanning electron microscopy, micrometer scale) and secondary ion mass spectrometry at the nanometer scale (nanoSIMS). The outcomes obtained in combination with findings from cooperation partners will help to unravel the contribution of different types of soil components on the formation and characteristics of the biogeochemical interfaces and their effect on organic chemical sorption.
Magnetic resonance tomography (MRT) on microcosm soil cores (200 mm Ø) used for CeMiX, comprising naturally stacked subsoil down to 700 mm plus topsoil from CeFiT, will be implemented at a laterally partially open Split 1.5 T magnet, with intended final in-plane spatial resolution of 200 Micro m. Three-dimensional biopore distributions and dynamics of their formation within the cores will be determined non-invasively and compared to complementing CT analyses of SP 2. One major aim is a non-invasive differentiation of the biopores into earthworm- and root system-originating ones and currently air-, water-, root- and earthwormfilled ones, based on NMR relaxation parameters. Attempts will additionally be made to classify different wall coatings of the biopores with regard to their water affinity. Dynamics of water distribution within the microcosm core and its biopore structures, starting from initial values taken from CeFiT (SP 3), will be documented with an in-plane resolution of 5 mm, in parallel to measurements of root growth dynamics for calculation of biomass and root surface area. Special emphasis will be put on the role of the plant root system for a re-distribution of water/D2O (and solutes) between different soil layers. Finally we will attempt MRT-controlled sample collection from the microcosm cores, to get - together with our research unit partners of SPs 4-8 - repeated access to minimally invasively acquired data on nutrient and microorganism distributions in concert with non-invasively collected water and root distribution data as a basis for dynamic modelling of water and solute circuits in SP 10. Beside the microcosm cores, flat rhizotrons as used in SP 3 will be employed to enable measurements of root and shoot hydrostatic pressure profiles with pressure probes, in addition to MRT measurements. In this way water distributions and corresponding driving forces and growth dynamics will be measured altogether in a minimally invasive manner.
Rain-cracking limits the production of many soft and fleshy fruit including sweet cherries world wide. Cracking is thought to result from increased water uptake through surface and pedicel. Water uptake increases fruit volume, and hence, turgor of cells (Pcell) and the pressure inside the fruit (Pfruit) and subjects the skin to tangential stress and hence, strain. When the strain exceeds the limits of extensibility the fruit cracks. This hypothesis is referred to as the Pfruit driven strain cracking. Based on this hypothesis cracking is related to two independent groups of factors: (1) water transport characteristics and (2) the intrinsic cracking susceptibility of the fruit defined as the amount of cracking per unit water uptake. The intrinsic cracking susceptibility thus reflects the mechanical constitution of the fruit. Most studies focussed on water transport through the fruit surface (factors 1), but only little information is available on the mechanical constitution (i.e., Pfruit and Pcell, tensile properties such as fracture strain, fracture pressure and modulus of elasticity of the exocarp; factors 2). The few published estimates of Pfruit in sweet cherry are all obtained indirectly (calculated from fruit water potential and osmotic potentials of juice extracts) and unrealistically high. They exceed those measured by pressure probe techniques in mature grape berry by several orders of magnitude. The objective of the proposed project is to test the hypothesis of the Pfruit driven strain cracking. Initially we will focus on establishing systems of widely differing intrinsic cracking susceptibility by varying species (sweet and sour cherry, Ribes and Vaccinium berries, plum, tomato), genotype (within sweet cherry), stage of development and temperature. These systems will then be used for testing the hypothesis of Pfruit driven strain cracking. We will quantify Pfruit und Pcell by pressure probe techniques and compression tests and the mechanical properties of the exocarp using biaxial tensile tests. When the presence of high Pfruit and Pcell is confirmed by direct measurements, subsequent studies will focus on the mode of failure of the exocarp (fracture along vs. across cell walls) and the relationship between failure thresholds and morphometric characteristics of the exocarp. However, when Pfruit und Pcell are low, the hypothesis of Pfruit driven strain cracking must be rejected and the mechanistic basis for low pressures (presence of apoplastic solutes) clarified on a temporal (in the course of development) and a spatial scale (exocarp vs. mesocarp). We focus on sweet cherry, because detailed information on this species and experience in extending the short harvest period is available. Where appropriate, other cracking susceptible species (sour cherry, plum, Vaccinium, Ribes, tomato) will be included to further extend the experimental period and to maximize the range in intrinsic cracking susceptibility.
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