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  • 1
    Language: English
    In: The Science of the Total Environment, Dec 1, 2015, Vol.535, p.35(10)
    Description: To link to full-text access for this article, visit this link: http://dx.doi.org/10.1016/j.scitotenv.2014.11.058 Byline: George Metreveli, Allan Philippe, Gabriele E. Schaumann Abstract: Silver nanoparticles (Ag NPs) could be found in aquatic systems in the near future. Although the interplay between aggregate formation and disaggregation is an important factor for mobility, bioavailability and toxicity of Ag NPs in surface waters, the factors controlling disaggregation of Ag NP homoaggregates are still unknown. In this study, we investigated the reversibility of homoaggregation of citrate coated Ag NPs in a Rhine River water matrix. We characterized the disaggregation of Ag NP homoaggregates by ionic strength reduction and addition of Suwannee River humic acid (SRHA) in the presence of strong and weak shear forces. In order to understand the disaggregation processes, we also studied the nature of homoaggregates and their formation dynamics under the influence of SRHA, Ca.sup.2+ concentration and nanoparticle concentration. Even in the presence of SRHA and at low particle concentrations (10[mu]gL.sup.-1), aggregates formed rapidly in filtered Rhine water. The critical coagulation concentration (CCC) of Ca.sup.2+ in reconstituted Rhine water was 1.5mmolL.sup.-1 and was shifted towards higher values in the presence of SRHA. Analysis of the attachment efficiency as a function of Ca.sup.2+ concentration showed that SRHA induces electrosteric stabilization at low Ca.sup.2+ concentrations and cation-bridging flocculation at high Ca.sup.2+ concentrations. Shear forces in the form of mechanical shaking or ultrasound were necessary for breaking the aggregates. Without ultrasound, SRHA also induced disaggregation, but it required several days to reach a stable size of dense aggregates still larger than the primary particles. Citrate stabilized Ag NPs may be in the form of reaction limited aggregates in aquatic systems similar to the Rhine River. The size and the structure of these aggregates will be dynamic and be determined by the solution conditions. Seasonal variations in the chemical composition of natural waters can result in a sedimentation-release cycle of engineered nanoparticles. Article History: Received 29 September 2014; Revised 16 November 2014; Accepted 16 November 2014
    Keywords: Water – Analysis ; Humic Acids – Analysis
    ISSN: 0048-9697
    Source: Cengage Learning, Inc.
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  • 2
    Language: English
    In: The Science of the Total Environment, Dec 1, 2015, Vol.535, p.54(7)
    Description: To link to full-text access for this article, visit this link: http://dx.doi.org/10.1016/j.scitotenv.2014.10.108 Byline: Sondra Klitzke, George Metreveli, Andre Peters, Gabriele E. Schaumann, Friederike Lang Abstract: Nanoparticles enter soils through various pathways. In the soil, they undergo various interactions with the solution and the solid phase. We tested the following hypotheses using batch experiments: i) the colloidal stability of Ag NP increases through sorption of soil-borne dissolved organic matter (DOM) and thus inhibits aggregation; ii) the presence of DOM suppresses Ag oxidation; iii) the surface charge of Ag NP governs sorption onto soil particles. Citrate-stabilized and bare Ag NPs were equilibrated with (colloid-free) soil solution extracted from a floodplain soil for 24h. Nanoparticles were removed through centrifugation. Concentrations of free Ag ions and DOC, the specific UV absorbance at a wavelength of 254nm, and the absorption ratio [alpha].sub.254/[alpha].sub.410 were determined in the supernatant. Nanoparticle aggregation was studied using time-resolved dynamic light scattering (DLS) measurement following the addition of soil solution and 1.5mM Ca.sup.2+ solution. To study the effect of surface charge on the adsorption of Ag NP onto soil particles, bare and citrate-stabilized Ag NP, differing in the zeta potential, were equilibrated with silt at a solid-to-solution ratio of 1:10 and an initial Ag concentration range of 30 to 320[mu]g/L. Results showed that bare Ag NPs sorb organic matter, with short-chained organic matter being preferentially adsorbed over long-chained, aromatic organic matter. Stabilizing effects of organic matter only come into play at higher Ag NP concentrations. Soil solution inhibits the release of Ag.sup.+ ions, presumably due to organic matter coatings. Sorption to silt particles was very similar for the two particle types, suggesting that the surface charge does not control Ag NP sorption. Besides, sorption was much lower than in comparable studies with sand and glass surfaces. Article History: Received 29 September 2014; Revised 30 October 2014; Accepted 30 October 2014 Article Note: (miscellaneous) Editor: D. Barcelo
    Keywords: Nanoparticles ; Adsorption
    ISSN: 0048-9697
    Source: Cengage Learning, Inc.
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  • 3
    Language: English
    In: The Science of the Total Environment, Dec 1, 2015, Vol.535, p.113(9)
    Description: To link to full-text access for this article, visit this link: http://dx.doi.org/10.1016/j.scitotenv.2015.03.023 Byline: Samuel K. Kumahor, Pavel Hron, George Metreveli, Gabriele E. Schaumann, Hans-Jorg Vogel Abstract: 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 1mM KNO.sub.3 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 3-5kT) 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. Article History: Received 9 December 2014; Revised 5 March 2015; Accepted 5 March 2015 Article Note: (miscellaneous) Editor: D. Barcelo
    Keywords: Nanoparticles – Analysis ; Multiprocessing – Analysis
    ISSN: 0048-9697
    Source: Cengage Learning, Inc.
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  • 4
    Language: English
    In: The Science of the Total Environment, Dec 1, 2015, Vol.535, p.1(2)
    Description: To link to full-text access for this article, visit this link: http://dx.doi.org/10.1016/j.scitotenv.2015.06.006 Byline: Gabriele E. Schaumann, Thomas Baumann, Friederike Lang, George Metreveli, Hans-Jorg Vogel
    Keywords: Soils
    ISSN: 0048-9697
    Source: Cengage Learning, Inc.
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  • 5
    Language: English
    In: Science of the Total Environment, 01 December 2015, Vol.535, pp.35-44
    Description: Silver nanoparticles (Ag NPs) could be found in aquatic systems in the near future. Although the interplay between aggregate formation and disaggregation is an important factor for mobility, bioavailability and toxicity of Ag NPs in surface waters, the factors controlling disaggregation of Ag NP homoaggregates are still unknown. In this study, we investigated the reversibility of homoaggregation of citrate coated Ag NPs in a Rhine River water matrix. We characterized the disaggregation of Ag NP homoaggregates by ionic strength reduction and addition of Suwannee River humic acid (SRHA) in the presence of strong and weak shear forces. In order to understand the disaggregation processes, we also studied the nature of homoaggregates and their formation dynamics under the influence of SRHA, Ca concentration and nanoparticle concentration. Even in the presence of SRHA and at low particle concentrations (10 μg L ), aggregates formed rapidly in filtered Rhine water. The critical coagulation concentration (CCC) of Ca in reconstituted Rhine water was 1.5 mmol L and was shifted towards higher values in the presence of SRHA. Analysis of the attachment efficiency as a function of Ca concentration showed that SRHA induces electrosteric stabilization at low Ca concentrations and cation-bridging flocculation at high Ca concentrations. Shear forces in the form of mechanical shaking or ultrasound were necessary for breaking the aggregates. Without ultrasound, SRHA also induced disaggregation, but it required several days to reach a stable size of dense aggregates still larger than the primary particles. Citrate stabilized Ag NPs may be in the form of reaction limited aggregates in aquatic systems similar to the Rhine River. The size and the structure of these aggregates will be dynamic and be determined by the solution conditions. Seasonal variations in the chemical composition of natural waters can result in a sedimentation-release cycle of engineered nanoparticles.
    Keywords: Coagulation Kinetics ; Aggregation ; Disaggregation ; Dls ; Natural Organic Matter ; Icp-MS ; Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 6
    Language: English
    In: Science of the Total Environment, 01 December 2015, Vol.535, pp.54-60
    Description: Nanoparticles enter soils through various pathways. In the soil, they undergo various interactions with the solution and the solid phase. We tested the following hypotheses using batch experiments: i) the colloidal stability of Ag NP increases through sorption of soil-borne dissolved organic matter (DOM) and thus inhibits aggregation; ii) the presence of DOM suppresses Ag oxidation; iii) the surface charge of Ag NP governs sorption onto soil particles. Citrate-stabilized and bare Ag NPs were equilibrated with (colloid-free) soil solution extracted from a floodplain soil for 24 h. Nanoparticles were removed through centrifugation. Concentrations of free Ag ions and DOC, the specific UV absorbance at a wavelength of 254 nm, and the absorption ratio α /α were determined in the supernatant. Nanoparticle aggregation was studied using time-resolved dynamic light scattering (DLS) measurement following the addition of soil solution and 1.5 mM Ca solution. To study the effect of surface charge on the adsorption of Ag NP onto soil particles, bare and citrate-stabilized Ag NP, differing in the zeta potential, were equilibrated with silt at a solid-to-solution ratio of 1:10 and an initial Ag concentration range of 30 to 320 μg/L. Results showed that bare Ag NPs sorb organic matter, with short-chained organic matter being preferentially adsorbed over long-chained, aromatic organic matter. Stabilizing effects of organic matter only come into play at higher Ag NP concentrations. Soil solution inhibits the release of Ag ions, presumably due to organic matter coatings. Sorption to silt particles was very similar for the two particle types, suggesting that the surface charge does not control Ag NP sorption. Besides, sorption was much lower than in comparable studies with sand and glass surfaces.
    Keywords: Isoelectric Point ; Cation Valency ; Initial Nanoparticle Concentration ; Exchangeability of Sorbed Ag Ions ; Environmental Sciences ; Biology ; Public Health
    ISSN: 0048-9697
    E-ISSN: 1879-1026
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  • 7
    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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  • 8
    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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  • 9
    Language: English
    In: PLoS ONE, 01 January 2018, Vol.13(6), p.e0199132
    Description: The application of engineered silver nanoparticles (AgNPs) in a considerable amount of registered commercial products inevitably will result in the continuous release of AgNPs into the natural aquatic environment. Therefore, native biofilms, as the prominent life form of microorganisms in almost all known ecosystems, will be subjected to AgNP exposure. Despite the exponentially growing research activities worldwide, it is still difficult to assess nanoparticle-mediated toxicity in natural environments. In order to obtain an ecotoxicologically relevant exposure scenario, we performed experiments with artificial stream mesocosm systems approaching low dose AgNP concentrations close to predicted environmental concentrations. Pregrown freshwater biofilms were exposed for 14 days to citrate-stabilized AgNPs at a concentration of 600 μg l-1 in two commonly used sizes (30 and 70 nm). Sublethal effects of AgNP treatment were assessed with regard to biofilm structure by gravimetric measurements (biofilm thickness and density) and by two biomass parameters, chlorophyll a and protein content. The composition of bacterial biofilm communities was characterized by t-RFLP fingerprinting combined with phylogenetic studies based on the 16S gene. After 14 days of treatment, the structural parameters of the biofilm such as thickness, density, and chlorophyll a and protein content were not statistically significantly changed by AgNP exposure. Furthermore, t-RFLP fingerprint analysis showed that the bacterial diversity was not diminished by AgNPs, as calculated by Shannon Wiener and evenness indices. Nevertheless, t-RFLP analysis also indicated that AgNPs led to an altered biofilm community composition as was shown by cluster analysis and multidimensional scaling (MDS) based on the Bray Curtis index. Sequence analysis of cloned 16S rRNA genes further revealed that changes in community composition were related with the displacement of putatively AgNP-sensitive bacterial taxa Actinobacteria, Chloroflexi, and Cyanobacteria by taxa known for their enhanced adaptability towards metal stress, such as Acidobacteria, Sphingomonadales, and Comamonadaceae. This measurable community shift, even after low dose AgNP treatment, causes serious concerns with respect to the broad application of AgNPs and their potentially adverse impact on the ecological function of lotic biofilms, such as biodegradation or biostabilization.
    Keywords: Sciences (General)
    E-ISSN: 1932-6203
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  • 10
    Language: English
    In: Aquatic Geochemistry, 2010, Vol.16(1), pp.85-100
    Description: In this work, the interaction of natural organic matter (NOM) with metal(loid)s (Cu, Pb, Zn, Pt, As) and the role of NOM on the metal(loid) transport in a water-saturated quartz sand column were investigated. For detailed information, size exclusion chromatographic (SEC) measurements and “short pulse” laboratory transport experiments with online metal(loid) and NOM detection were used. The SEC measurements showed the formation of metal–NOM complexes. Cu, Pb, Zn and Pt were predominantly bound to the high molecular mass NOM molecules. The binding capacity of the NOM for metals increased with increasing pH value and in the following order: Zn 〈 Pb 〈 Cu 〈 Pt. No evidence for the formation of As–NOM complexes was found. The transport experiments showed no significant influence of NOM on the mobility of Cu, Pb and Zn. The metal–NOM complexes detected in the SEC experiments were obviously sorbed completely onto the grain surfaces in case of the quartz sand system, or they were dissociated partially during passage through the column. No influence of NOM was observed on the transport of As as well. Inorganic Zn and As species were transported through the column with increasing retardation as the pH value increased. Pt showed a high mobility at a pH of 5, and it decreased at a pH of 7 especially in the presence of NOM. The results support the known fact that a decrease in the pH value results in enhanced transport of inorganic metal(loid) species in water-saturated porous media. On the other hand, the presence of NOM can immobilise the metals through metal–NOM complex formation and the deposition of the complexes onto the stationary phase.
    Keywords: NOM ; Metal(loid)s ; SEC ; Transport experiments ; Porous media
    ISSN: 1380-6165
    E-ISSN: 1573-1421
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