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  • Vogel, Hans-Jorg  (15)
  • Elsevier (CrossRef)  (15)
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  • 1
    Language: English
    In: Science of the Total Environment, 01 December 2015, Vol.535, pp.3-19
    Description: Engineered inorganic nanoparticles (EINP) from consumers' products and industrial applications, especially silver and titanium dioxide nanoparticles (NP), are emitted into the aquatic and terrestrial environments in increasing amounts. However, the current knowledge on their environmental fate and biological effects is diverse and renders reliable predictions complicated. This review critically evaluates existing knowledge on colloidal aging mechanisms, biological functioning and transport of Ag NP and TiO NP in water and soil and it discusses challenges for concepts, experimental approaches and analytical methods in order to obtain a comprehensive understanding of the processes linking NP fate and effects. Ag NP undergo dissolution and oxidation with Ag S as a thermodynamically determined endpoint. Nonetheless, Ag NP also undergo colloidal transformations in the nanoparticulate state and may act as carriers for other substances. Ag NP and TiO NP can have adverse biological effects on organisms. Whereas Ag NP reveal higher colloidal stability and mobility, the efficiency of NOM as a stabilizing agent is greater towards TiO NP than towards Ag NP, and multivalent cations can dominate the colloidal behavior over NOM. Many of the past analytical obstacles have been overcome just recently. Single particle ICP-MS based methods in combination with field flow fractionation techniques and hydrodynamic chromatography have the potential to fill the gaps currently hampering a comprehensive understanding of fate and effects also at a low field relevant concentrations. These analytical developments will allow for mechanistically orientated research and transfer to a larger set of EINP. This includes separating processes driven by NP specific properties and bulk chemical properties, categorization of effect-triggering pathways directing the EINP effects towards specific recipients, and identification of dominant environmental parameters triggering fate and effect of EINP in specific ecosystems (e.g. soil, lake, or riverine systems).
    Keywords: Transport ; Aggregation ; Analytics ; Environment ; Aging ; Ecotoxicology ; Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 2
    Language: English
    In: Science of the Total Environment, 01 December 2015, Vol.535, pp.1-2
    Keywords: Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 3
    Language: English
    In: Science of the Total Environment, 01 December 2015, Vol.535, pp.113-121
    Description: Chemical factors and physical constraints lead to coupled effects during particle transport in unsaturated porous media. Studies on unsaturated transport as typical for soils are currently scarce. In unsaturated porous media, particle mobility is determined by the existence of an air–water interface in addition to a solid–water interface. To this end, we measured breakthrough curves and retention profiles of citrate-coated Ag nanoparticles in unsaturated sand at two pH values (5 and 9) and three different flow rates corresponding to different water contents with 1 mM KNO as background electrolyte. The classical DLVO theory suggests unfavorable deposition conditions at the air–water and solid–water interfaces. The breakthrough curves indicate modification in curve shapes and retardation of nanoparticles compared to inert solute. Retention profiles show sensitivity to flow rate and pH and this ranged from almost no retention for the highest flow rate at pH = 9 to almost complete retention for the lowest flow rate at pH = 5. Modeling of the breakthrough curves, thus, required coupling two parallel processes: a kinetically controlled attachment process far from equilibrium, responsible for the shape modification, and an equilibrium sorption, responsible for particle retardation. The non-equilibrium process and equilibrium sorption are suggested to relate to the solid–water and air–water interfaces, respectively. This is supported by the DLVO model extended for hydrophobic interactions which suggests reversible attachment, characterized by a secondary minimum (depth 3–5 kT) and a repulsive barrier at the air–water interface. In contrast, the solid–water interface is characterized by a significant repulsive barrier and the absence of a secondary minimum suggesting kinetically controlled and non-equilibrium interaction. This study provides new insights into particle transport in unsaturated porous media and offers a model concept representing the relevant processes.
    Keywords: Air–Water Interface ; Solid–Water Interface ; Engineered Nanoparticle ; Extended Dlvo Theory ; Unsaturated Flow ; Pore Structure ; Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 4
    Language: English
    In: Ecological Modelling, 24 February 2015, Vol.298, pp.1-3
    Keywords: Environmental Sciences ; Ecology
    ISSN: 0304-3800
    E-ISSN: 1872-7026
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  • 5
    Language: English
    In: Science of the Total Environment, 15 December 2018, Vol.645, pp.192-204
    Description: Riverbank filtration systems are important structures that ensure the cleaning of infiltrating surface water for drinking water production. In our study, we investigated the potential risk for a breakthrough of environmentally aged silver nanoparticles (Ag NP) through these systems. Additionally, we identified factors leading to the remobilization of Ag NP accumulated in surficial sediment layers in order to gain insights into remobilization mechanisms. We conducted column experiments with Ag NP in an outdoor pilot plant consisting of water-saturated sediment columns mimicking a riverbank filtration system. The NP had previously been aged in river water, soil extract, and ultrapure water, respectively. We investigated the depth-dependent breakthrough and retention of NP. In subsequent batch experiments, we studied the processes responsible for a remobilization of Ag NP retained in the upper 10 cm of the sediments, induced by ionic strength reduction, natural organic matter (NOM), and mechanical forces. We determined the amount of remobilized Ag by ICP-MS and differentiated between particulate and ionic Ag after remobilization using GFAAS. The presence of Ag-containing heteroaggregates was investigated by combining filtration with single-particle ICP-MS. Single and erratic Ag breakthrough events were mainly found in 30 cm depth and Ag NP were accumulated in the upper 20 cm of the columns. Soil-aged Ag NP showed the lowest retention of only 54%. Remobilization was induced by the reduction of ionic strength and the presence of NOM in combination with mechanical forces. The presence of calcium in the aging- as well as the remobilizing media reduced the remobilization potential. Silver NP were mainly remobilized as heteroaggregates with natural colloids, while dissolution played a minor role. Our study indicates that the breakthrough potential of Ag NP in riverbank filtration systems is generally low, but the aging in soil increases their mobility. Remobilization processes are associated to co-mobilization with natural colloids.
    Keywords: Heteroaggregation ; Nanoparticle Transformation ; Breakthrough ; Mobility ; Reversibility ; Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 6
    Language: English
    In: Advances in Water Resources, August 2012, Vol.44, pp.101-112
    Description: ► New averaging approach that conserves hydraulic non-equilibrium during rapid infiltration of water. ► New indicators to describe hydraulic non-equilibrium quantitatively. ► Direct link between front morphology and hydraulic non-equilibrium. ► Insights into how structural connectivity affects hydraulic non-equilibrium. ► Shortcomings of an upscaled Richards model extended by hydraulic non-equilibrium. Water infiltration into heterogeneous, structured soil leads to hydraulic non-equilibrium across the infiltration front. That is, the water content and pressure head are not in equilibrium according to some static water retention curve. The water content increases more rapidly in more conductive regions followed by a slow relaxation towards an equilibrium state behind the front. An extreme case is preferential infiltration into macropores. Since flow paths adapt to the structural heterogeneity of the porous medium, there is a direct link between structure and non-equilibrium. The aim of our study is to develop an upscaled description of water dynamics which conserves the macroscopic effects of non-equilibrium and which can be directly linked to structural properties of the material. A critical question is how to define averaged state variables at the larger scale. We propose a novel approach based on flux-weighted averaging of pressure head, and compare its performance to alternative methods for averaging. Further, we suggest some meaningful indicators of hydraulic non-equilibrium that can be related to morphological characteristics of infiltration fronts in quantitative terms. These methods provide a sound basis to assess the impact of structural connectivity on hydraulic non-equilibrium. We demonstrate our approach using numerical case studies for infiltration into two-dimensional heterogeneous media using three different structure models with distinct differences in connectivity. Our results indicate that an increased isotropic, short-range connectivity reduces non-equilibrium, whereas anisotropic structures that are elongated in the direction of flow enforce it. We observe a good agreement between front morphology and effective hydraulic non-equilibrium. A detailed comparison of averaged state variables with results from an upscaled model that includes hydraulic non-equilibrium outlines potential improvements in the description of non-equilibrium dynamics including preferential flow in simplified, upscaled models based on Richards equation.
    Keywords: Transient Flow ; Upscaling ; Pressure Head Averaging ; Hydraulic Non-Equilibrium ; Preferential Flow ; Connectivity ; Engineering
    ISSN: 0309-1708
    E-ISSN: 1872-9657
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  • 7
    Language: English
    In: Soil & Tillage Research, January 2018, Vol.175, pp.205-216
    Description: In recent years, there has been an increased application of conservation-oriented tillage techniques, where instead of being turned the soil is only loosened or not tilled at all. Strip tillage, a special form of conservation tillage, results in small-scale structural differences, since tillage is performed only within the seed row, while the soil between seed rows is not tilled. However, tillage always impacts upon physical soil properties and processes. A combined application of conventional soil mechanical methods and X-ray computed tomography (X-ray CT) is employed here in order to investigate small-scale structural differences in a chernozem (texture 0–30 cm: silt loam) located in central Germany under strip tillage (within and between seed rows) compared to no tillage and mulch tillage. Apart from recording changes over time (years: 2012, 2014, 2015) to dry bulk density and saturated conductivity at soil depths 2–8 and 12–18 cm, stress-strain tests were conducted to map mechanical behaviour for a load range of 5–550 kPa at a soil depth of 12–18 cm (year 2015). Mechanical precompression stress was determined from the stress-dry bulk density curves. In addition, computed tomography scans were created followed by quantitative image analysis of the morphometric parameters mean macropore diameter, macroporosity, connectivity and anisotropy of the same soil samples. For strip tillage between seed rows and no tillage, a significant increase in dry bulk density was observed over time compared to strip tillage within the seed row and mulch tillage. This was more pronounced at a soil depth of 2–8 cm than at 12–18 cm. Despite higher dry bulk density, strip tillage between the seed row displayed also an increasing saturated conductivity compared to strip tillage within the seed row and mulch tillage. The computed tomography scans showed that the macropores became more compressed and soil aggregates were pushed together as mechanical stress increased, with the aggregate arrangement being transformed down into a coherent soil mass. The soil mechanical and morphometric parameters supported each other in terms of what they revealed about the mechanical properties of the soil structures. For instance, in the strip tillage between seed rows and no tillage treatments, the lack of soil tillage not only resulted in higher dry bulk densities, but also higher aggregate densities, mechanical precompression stress values, mean macropore diameters as well as lower macroporosity and connectivity values compared to mulch tillage and strip tillage within the seed row. The computed tomography parameters are therefore highly suitable for providing Supplementary information about the compaction process. Overall, this study showed that strip tillage combines the advantages of no tillage and a deeper, soil conservation-oriented primary tillage because, on a small scale, it creates two distinct soil structures which are beneficial in terms of optimal plant growth as well as mechanical resistance by driving over the soil.
    Keywords: Pre-Compression Stress ; Dry Bulk Density ; Aggregate Density ; Image Analysis ; Soil Compaction ; Agriculture
    ISSN: 0167-1987
    E-ISSN: 1879-3444
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  • 8
    Language: English
    In: Geoderma, 01 September 2018, Vol.325, pp.37-48
    Description: Organic particles including microorganisms are a significant fraction of the mobile organic matter (MOM) pool that contributes to initial pedogenesis. Still, the dynamics and the interplay of the multitude of processes that control the mobilization, transport, and retention of MOM are vastly unclear. We studied this interplay using an ‘artificial soil’ as model for a young, unstructured soil with defined initial composition employing a novel two-layer column experiment. The upstream layer was composed of a mixture of well-defined mineral phases, a sterile organic matter source and a diverse, natural microbial inoculant mimicking an organic-rich topsoil. The downstream layer, mimicking the subsoil, was composed of the mineral phases, only. Columns were run under water-unsaturated flow conditions with multiple flow interruptions to reflect natural flow regimes and to detect possible non-equilibrium processes. Pore system changes caused by flow were inspected by scanning electron microscopy and computed micro-tomography. MOM-related physicochemical effluent parameters and bacterial community diversity and abundance were assessed by molecular analysis of the effluent and the solid phase obtained after the long-term irrigation experiment (75 d). Tomographic data showed homogeneous packing of the fine-grained media (sandy loam). During flow, the initially single-grain structured artificial soil showed no connected macropores. In total, 6% of the initial top layer organic matter was mobile. The release and transport of particulate (1.2%) and dissolved organic matter (4.8%) including bacteria were controlled by non-equilibrium conditions. Bacterial cells were released and selectively transported to downstream layer resulting in a depth-dependent and selective establishment of bacterial communities in the previously sterile artificial soil. This study underlines the importance of bacterial transport from the surface or topsoil for colonization and maturation of downstream compartments. This initial colonization of pristine surfaces is the major step in forming biogeochemical interfaces - the prominent locations of intensive biological activity and element turnover that seem to play a major role for the functioning of soil.
    Keywords: Mobile Organic Matter ; Unsaturated Two-Layer Column Experiment ; Experimental Pedogenesis ; Artificial Soil ; Computed Micro-Tomography ; Molecular Analysis ; Agriculture
    ISSN: 0016-7061
    E-ISSN: 1872-6259
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  • 9
    Language: English
    In: Journal of Contaminant Hydrology, December 2016, Vol.195, pp.31-39
    Description: Engineered nanoparticles released into soils may be coated with humic substances, potentially modifying their surface properties. Due to their amphiphilic nature, humic coating is expected to affect interaction of nanoparticle at the air-water interface. In this study, we explored the roles of the air-water interface and solid-water interface as potential sites for nanoparticle attachment and the importance of hydrophobic interactions for nanoparticle attachment at the air-water interface. By exposing Ag nanoparticles to soil solution extracted from the upper soil horizon of a floodplain soil, the mobility of the resulting “soil-aged” Ag nanoparticles was investigated and compared with the mobility of citrate-coated Ag nanoparticles as investigated in an earlier study. The mobility was determined as a function of hydrologic conditions and solution chemistry using column breakthrough curves and numerical modeling. Specifically, we compared the mobility of both types of nanoparticles for different unsaturated flow conditions and for pH = 5 and pH = 9. The soil-aged Ag NP were less mobile at pH = 5 than at pH = 9 due to lower electrostatic repulsion at pH = 5 for both types of interfaces. Moreover, the physical flow field at different water contents modified the impact of chemical forces at the solid-water interface. An extended Derjaguin-Landau-Verwey-Overbeek (eDLVO) model did not provide satisfactory explanation of the observed transport phenomena unlike for the citrate-coated case. For instance, the eDLVO model assuming sphere-plate geometry predicts a high energy barrier (〉 90 ) for the solid-water interface, indicating that nanoparticle attachment is less likely. Furthermore, retardation through reversible sorption at the air-water interface was probably less relevant for soil-aged nanoparticles than for citrate-coated nanoparticles. An additional cation bridging mechanism and straining within the flow field may have enhanced nanoparticle retention at the solid-water interface. The results indicate that the mobility of engineered Ag nanoparticles is sensitive to solution chemistry, especially pH and the concentration of multivalent cations, and to the unsaturated flow conditions influencing particle interaction at biogeochemical interfaces.
    Keywords: Unsaturated Transport ; Water Dynamics ; Cation Bridging ; Amphiphilic ; Edlvo ; Engineering ; Environmental Sciences ; Geography
    ISSN: 0169-7722
    E-ISSN: 1873-6009
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  • 10
    Language: English
    In: Geoderma, 01 July 2019, Vol.345, pp.63-71
    Description: Soil structure is not static but undergoes continuous changes due to a wide range of biotic and abiotic drivers such as bioturbation and the mechanical disturbance by tillage. This continuous alteration of soil structure beyond the pure swelling and shrinking of some stable structure is what we refer to as soil structure dynamics. It has important consequences for carbon turnover in soil as it controls how quickly soil organic matter gets occluded from or exposed to mineralization. So far there are hardly any direct observations of the rate at which soil pores are formed and destroyed. Here we employ are recently introduced labeling approach for soil structure that measures how quickly the locations of small garnet particles get randomized in soil as a measure for soil structure dynamics. We investigate the effect of desiccation crack dynamics on pore space attributes in general and soils structure turnover in particular using X-ray microtomography for repeated wetting-drying cycles. This is explored for three different soils with a range of soil organic matter content, clay content and different clay mineralogy that were sieved to a certain aggregate size fraction (0.63–2 mm) and repacked at two different bulk density levels. The total magnitude of desiccation crack formation mainly depended on the clay content and clay mineralogy. Higher soil organic matter content led to a denser crack pattern with smaller aperture. Wetting-drying cycles did not only effect visible macroporosity (〉8 μm), but also unresolved mesoporosity. The changes in macroporosity were higher at lower bulk density. Most importantly, repeated wetting-drying cycles did not lead to a randomization of distances between garnet particles and pores. This demonstrates that former failure zones are reactivated during subsequent drying cycles. Hence, wetting-drying resulted in reversible particle displacement and therefore would not have triggered the exposure of occluded carbon that was not already exposed during the previous drying event.
    Keywords: Soil Structure ; Desiccation Cracks ; X-Ray Tomography ; Macropores ; Clay Mineralogy ; Carbon Turnover ; Agriculture
    ISSN: 0016-7061
    E-ISSN: 1872-6259
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