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  • Transport
  • 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.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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  • 3
    Language: English
    In: Advances in Water Resources, 2011, Vol.34(2), pp.314-325
    Description: ► Stochastic reconstruction with a combination of multi-point statistics. ► Good rendition of connectivity with Minkowski functions and Chord length distributions. ► Transport behavior compares well between reference media and reconstructed media. ► Pressure field tends to bridge local discontinuities within highly conductive regions. Flow and transport in porous media is determined by its structure. Beside spatial correlation, especially the connectivity of heterogeneous conductivities is acknowledged to be a key factor. This has been demonstrated for well defined random fields having different topological properties. Yet, it remains an open question which morphological measures carry sufficient information to actually predict flow and transport in porous media. We analyze flow and transport in classical, two-dimensional random fields showing different topology and we determine a selection of structural characteristics including classical two-point statistics, chord-length distribution and Minkowski functions (four-point statistics) including the Euler number as a topological measure. Using the approach of simulated annealing for global optimization we generate analog random fields that are forced to reproduce one or several of theses structural characteristics. Finally we evaluate in how far the generated analogons reproduce the original flow and transport behavior as well as some more elaborate structural characteristics including percolation probabilities and the pair connectivity function. The results confirm that two-point statistics is insufficient to capture functional properties since it is not sensitive to connectivity. In contrast, the combination of Minkowski functions and chord length distributions carries sufficient information to reproduce the breakthrough curve of a conservative solute. Hence, global topology provided by the Euler number together with local clustering provided by the chord length distribution seems to be a powerful condensation of structural complexity with respect to functional properties.
    Keywords: Simulated Annealing ; Solute Transport ; Minkowski Functionals ; Chord Length Distribution ; Local Percolation Probability ; Pair Connectivity Function ; Engineering
    ISSN: 0309-1708
    E-ISSN: 1872-9657
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  • 4
    Language: English
    In: Vadose Zone Journal, 2012, Vol.11(3), p.0
    Description: Recently, a new approach was introduced to directly measure unsaturated hydraulic conductivity in flux-controlled experiments--the multistep flux experiment. Thereby an overshoot in matric potential h (sub m) across drainage and infiltration fronts was observed. We extended this experimental approach to simultaneously measure the volumetric water content Theta within the sample and applied the method to a sand and a clay loam soil. The detailed trajectories within the h (sub m) -Theta space were obtained during a number of decreasing and increasing steps in infiltration rate. This clearly demonstrates the type and magnitude of hydraulic nonequilibrium under transient conditions where water content and matric potential deviate from a well-defined static relation. We also compared the directly measured hydraulic conductivities with those obtained from classical multistep outflow experiments and found that nonequilibrium dynamics might lead to an underestimation of hydraulic conductivity when obtained from an inverse solution of Richards" equation. We provide a qualitative explanation of nonequilibrium that depends on the structure of the material and the type and magnitude of external forcing. The new experimental setup is considered to be a valuable tool to actually quantify nonequilibrium effects. This will make it possible to represent this relevant phenomenon in future modeling concepts.
    Keywords: Hydrogeology ; Aquifers ; Climate Forcing ; Discharge ; Drainage ; Experimental Studies ; Ground Water ; Hydraulic Conductivity ; Hydrodynamics ; Hysteresis ; Infiltration ; Models ; Richards Equation ; Saturation ; Soil Mechanics ; Solute Transport ; Transport ; Unsaturated Zone;
    ISSN: Vadose Zone Journal
    E-ISSN: 1539-1663
    Source: CrossRef
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  • 5
    Language: English
    In: Vadose Zone Journal, 2011, Vol.10(3), p.1082
    Description: Predicting solute transport through structured soil based on observable structural properties of the material has not been accomplished to date. We evaluated a new approach to predicting breakthrough curves (BTCs) of dissolved chemicals in intact structured soil columns based on attributes of the pore structure at hierarchical spatial scales. The methodology centers on x-ray computed microtomography of a hierarchic suite of undisturbed soil samples (diameters 1, 4.6, 7.5, and 16 cm) to identify the network of pores 〉10 mu m in diameter. The pore structure was quantified in terms of pore size distribution, interface area density, and connectivity. The pore size distribution and pore connectivity were used to set up an equivalent pore network model (PNM) for predicting the BTCs of Br (super -) and Brilliant Blue FCF (BB) at unsaturated, steady-state flux. For a structured silt loam soil column, the predictions of Br (super -) tracer breakthrough were within the variation observed in the column experiments. A similarly good prediction was obtained for Br (super -) breakthrough in a sandy soil column. The BB breakthrough observed in the silt loam was dominated by a large variation in sorption (retardation factors between R = 2.9 and 24.2). The BB sorption distribution coefficient, k (sub d) , was measured in batch tests. Using the average k (sub d) in the PNM resulted in an overestimated retardation (R = 28). By contrast, breakthrough of BB in the sandy soil (experimental R = 3.3) could be roughly predicted using the batch test k (sub d) (PNM simulation R = 5.3). The prediction improved when applying a sorption correction function accounting for the deviation between measured interface area density distribution and its realization in the network model (R = 4.1). Overall, the results support the hypothesis that solute transport can be estimated based on a limited number of characteristics describing pore structure: the pore size distribution, pore topology, and pore-solid interfacial density.
    Keywords: Soils ; Bad Lauchstadt Germany ; Boundary Conditions ; Breakthrough Curves ; Bromine ; Central Europe ; Central Germany ; Chemical Dispersion ; Chernozems ; Computed Tomography ; Convection ; Density ; Dye Tracers ; Equations ; Europe ; Experimental Studies ; Fuhrberg Germany ; Germany ; Halogens ; Image Analysis ; Laboratory Studies ; Lower Saxony Germany ; Microtomography ; Minckowski Functions ; Morphology ; Networks ; Podzols ; Porosity ; Quantitative Analysis ; Saxony-Anhalt Germany ; Simulation ; Soils ; Solute Transport ; Spectra ; Tomography ; Topology ; Transport ; X-Ray Spectra;
    ISSN: Vadose Zone Journal
    E-ISSN: 1539-1663
    Source: CrossRef
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  • 6
    In: Water Resources Research, November 2018, Vol.54(11), pp.9033-9044
    Description: Structural hierarchy is a fundamental characteristic of natural porous media. Yet it provokes one of the grand challenges for the modeling of fluid flow and transport since pore‐scale structures and continuum‐scale domains often coincide independent of the observation scale. Common approaches to represent structural hierarchy build, for example, on a multidomain continuum for transport or on the coupling of the Stokes equations with Darcy's law for fluid flow. These approaches, however, are computationally expensive or introduce empirical parameters that are difficult to derive with independent observations. We present an efficient model for fluid flow based on Darcy's law and the law of Hagen‐Poiseuille that is parameterized based on the explicit pore space morphology obtained, for example, by X‐ray μ‐CT and inherently permits the coupling of pore‐scale and continuum‐scale domain. We used the resulting flow field to predict the transport of solutes via particle tracking across the different domains. Compared to experimental breakthrough data from laboratory‐scale columns with hierarchically structured porosity built from solid glass beads and microporous glass pellets, an excellent agreement was achieved without any calibration. Furthermore, we present different test scenarios to compare the flow fields resulting from the Stokes‐Brinkman equations and our approach to comprehensively illustrate its advantages and limitations. In this way, we could show a striking efficiency and accuracy of our approach that qualifies as general alternative for the modeling of fluid flow and transport in hierarchical porous media, for example, fractured rock or karstic aquifers. A model for the simulation of pore‐scale and continuum‐scale flow in hierarchically structured porous media is developed Explicit pore space morphology obtained by image analysis of X‐ray micro‐CT images is used for parameterization Predictions of solute breakthrough obtained by particle tracking perfectly match observations
    Keywords: Darcy'S Law ; Particle Tracking ; Column Experiments ; X‐Ray Μ‐Ct ; Pore Space Morphology ; Image Analysis
    ISSN: 0043-1397
    E-ISSN: 1944-7973
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  • 7
    In: Ecohydrology, September 2018, Vol.11(6), pp.n/a-n/a
    Description: By applying the newly developed flow cell (FC) concept, this study investigated the impact of small‐scale spatial variations (millimetre to centimetre) in organic matter (OM) composition (diffusive reflectance infrared Fourier transform spectroscopy), biological activity (zymography), and wettability (contact angle [CA]) on transport processes (tracer experiments, radiography). Experiments were conducted in five undisturbed soil slices (millimetre apart), consisting of a sandy matrix with an embedded loamy band. In the loamy band increased enzyme activities and OM (10 mm apart) were found compared with the sand matrix, with no interrelations although spatial autocorrelation ranges were up to 7 cm. CAs were increased (0–110°) above the loamy band and were negatively correlated with acid phosphatase. Missing correlations were probably attributed to texture variations between soil slices. A general correlation between CA and C content (bulk) were confirmed. Variability in texture and hydraulic properties led to the formation of heterogeneous flow patterns and probably to heterogeneously distributed interfacial properties. The new FC concept allows process evaluation on the millimetre scale to analyse spatial relations, that is, between small‐scale textural changes on transport processes and biological responses. The concept has been proved as a versatile tool to analyse spatial distribution of biological and interfacial soil properties in conjunction with the analysis of complex micro‐hydraulic processes for undisturbed soil samples. The concept may be improved by additional nondestructive imaging methods, which is especially challenging for the detection of small‐scale textural changes.
    Keywords: Drift Spectroscopy ; Extracellular Enzyme Activity ; Flow Cell ; Soil Water Repellency ; Transport Processes ; Undisturbed Soil ; X‐Ray Radiography
    ISSN: 1936-0584
    E-ISSN: 1936-0592
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  • 8
    Language: English
    In: Soil Science Society of America Journal, 2013, Vol.77(2), p.403
    Description: The influence of clay content in soil-pore structure development and the relative importance of macroporosity in governing convective fluid flow are two key challenges toward better understanding and quantifying soil ecosystem functions. In this study, soil physical measurements (soil-water retention and air permeability) and x-ray computed tomography (CT) scanning were combined and used from two scales on intact soil columns (100 and 580 cm super(3)). The columns were sampled along a natural clay gradient at six locations (L1, L2, L3, L4, L5 and L6 with 0.11, 0.16, 0.21, 0.32, 0.38 and 0.46 kg kg super(-1) clay content, respectively) at a field site in Lerbjerg, Denmark. The water-holding capacity of soils markedly increased with increasing soil clay content, while significantly higher air permeability was observed for the L1 to L3 soils than for the L4 to L6 soils. Higher air permeability values observed for 580- than 100-cm super(3) soil columns implied a scale effect and relatively greater importance of macropores in convective fluid flow at larger scale. Supporting this, x-ray CT showed that both interaggregate pores and biopores (pores formed by earthworms and plant roots) were present at L1 to L3 in decreasing order, whereas only interaggre- gate pores were observed at L4 to L6. Macroporosity inferred from x-ray CT to quantify pores 1 mm decreased from 2.9 to 0.1 % from L1 to L6. A progressive improvement was observed in the linear relationship (R super(2) increasing 0.50-0.95) of air permeability with total air-filled porosity, CT-inferred macroporosity, and CT-inferred limiting macroporosity (minimum macroporosity for any quarter of soil column). The findings of this study show the immense potential in linking x-ray CT-derived soil-pore parameters with classical soil physical measurements for quantifying soil architecture and functions. [PUBLICATION]
    Keywords: Soil ; Permeability ; Earthworms ; Soil Structure ; Clay ; Porosity ; Computed Tomography ; Denmark ; Air Pollution;
    ISSN: Soil Science Society of America Journal
    E-ISSN: 0361-5995
    E-ISSN: 14350661
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  • 9
    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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  • 10
    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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