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• Vogel, Hans-Jorg  (32)
• Vogel, H.-J.  (32)
• 1
Article
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
Article
Language: English
In: PLoS ONE, 01 January 2016, Vol.11(7), p.e0159948
Description: Matter turnover in soil is tightly linked to soil structure which governs the heterogeneous distribution of habitats, reaction sites and pathways in soil. Thereby, the temporal dynamics of soil structure alteration is deemed to be important for essential ecosystem functions of soil but very little is known about it. A major reason for this knowledge gap is the lack of methods to study soil structure turnover directly at microscopic scales. Here we devise a conceptual approach and an image processing workflow to study soil structure turnover by labeling some initial state of soil structure with small garnet particles and tracking their fate with X-ray microtomography. The particles adhere to aggregate boundaries at the beginning of the experiment but gradually change their position relative to the nearest pore as structure formation progresses and pores are destructed or newly formed. A new metric based on the contact distances between particles and pores is proposed that allows for a direct quantification of soil structure turnover rates. The methodology is tested for a case study about soil compaction of a silty loam soil during stepwise increase of bulk density (ρ = {1.1, 1.3, 1.5} g/cm3). We demonstrate that the analysis of mean contact distances provides genuinely new insights about changing diffusion pathways that cannot be inferred neither from conventional pore space attributes (porosity, mean pore size, pore connectivity) nor from deformation analysis with digital image correlation. This structure labeling approach to quantify soil structure turnover provides a direct analogy to stable isotope labeling for the analysis of matter turnover and can be readily combined with each other.
Keywords: Sciences (General)
E-ISSN: 1932-6203
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• 3
Article
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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• 4
Article
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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• 5
Article
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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• 6
Article
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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• 7
Article
Language: English
In: Transport in Porous Media, 2016, Vol.112(1), pp.207-227
Description: According to experimental observations, capillary trapping is strongly dependent on the roughness of the pore–solid interface. We performed imbibition experiments in the range of capillary numbers ( Ca ) from $$10^{-6}$$ 10 - 6 to $$5\times 10^{-5}$$ 5 × 10 - 5 using 2D-micromodels, which exhibit a rough surface. The microstructure comprises a double-porosity structure with pronounced macropores. The dynamics of precursor thin-film flow and its importance for capillary trapping are studied. The experimental data for thin-film flow advancement show a square-root time dependence. Based on the experimental data, we conducted inverse modeling to investigate the influence of surface roughness on the dynamic contact angle of precursor thin-film flow. Our experimental results show that trapped gas saturation decreases logarithmically with an increasing capillary number. Cluster analysis shows that the morphology and number of trapped clusters change with capillary number. We demonstrate that capillary trapping shows significant differences for vertical flow and horizontal flow. We found that our experimental results agree with theoretical results of percolation theory for $$Ca =10^{-6}$$ C a = 10 - 6 : (i) a universal power-like cluster size distribution, (ii) the linear surface–volume relationship of trapped clusters, and (iii) the existence of the cutoff correlation length for the maximal cluster height. The good agreement is a strong argument that the experimental cluster size distribution is caused by a percolation-like trapping process (ordinary percolation). For the first time, it is demonstrated experimentally that the transition zone model proposed by Wilkinson (Phys Rev A 30:520–531, 1984) can be applied to 2D-micromodels, if bicontinuity is generalized such that it holds for the thin-film water phase and the bulk gas phase.
Keywords: 2D-micromodel with rough surface ; Precursor thin-film flow ; Snap-off trapping ; Universal power law ; Ordinary bond percolation
ISSN: 0169-3913
E-ISSN: 1573-1634
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• 8
Article
Language: English
In: Vadose Zone Journal, 2015, Vol.14(5), p.0
Description: The guest editors introduce the seven contributions to the special issue on processes in capillary fringes, with a focus on the complex interaction of biological, chemical, and physical processes in this environemnt. Processes in capillary fringes (CFs) have a complex nature due to the interactions between the solid, liquid, and gaseous environments. Despite a considerable body of literature on CFs coming from different disciplines, the ongoing processes and their complex interactions are yet only partially understood.
Keywords: Soils ; Solids ; Vadose Water ; Methods and Instruments ; General;
E-ISSN: 1539-1663
Source: CrossRef
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• 9
Article
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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• 10
Article
Language: English
In: Vadose Zone Journal, 2015, Vol.14(5), p.0
Description: We used X-ray computed microtomography to study gas trapping in a fluctuating water table. Our results show that capillary forces control trapping and phase distribution in dynamic capillary fringes. In porous media, the nonwetting phase is trapped on water saturation due to capillary forces acting in a heterogeneous porous structure. Within the capillary fringe, the gas phase is trapped and released along with the fluctuation of the water table, creating a highly active zone for biological transformations and mass transport. We conducted column experiments to observe and quantify the magnitude and structure of the trapped gas phase at the pore scale using computed microtomography. Different grain size distributions of glass beads were used to study the effect of the pore structure on trapping at various capillary numbers. Viscous forces were found to have negligible impact on phase trapping compared with capillary and buoyancy forces. Residual gas saturations ranged from 0.5 to 10%, while residual saturation increased with decreasing grain size. The gas phase was trapped by snap-off in single pores but also in pore clusters, while this single-pore trapping was dominant for grains larger than 1 mm in diameter. Gas surface area was found to increase linearly with increasing gas volume and with decreasing grain size.
Keywords: Grain Size ; Water Table ; Mass Transport ; Buoyancy ; Pores ; Porous Media ; Particle Size ; Water Table ; Saturation ; Vadose Water ; Fluctuations ; Trapping ; Buoyancy ; Methods and Instruments ; General;