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| 2. |
- Apul, Defne S., et al.
(författare)
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Geochemical Modeling of Trace Element Release from Biosolids
- 2010
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Ingår i: Environmental Engineering Science. - : Mary Ann Liebert. - 1092-8758 .- 1557-9018. ; 27:9, s. 743-755
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Tidskriftsartikel (refereegranskat)abstract
- Biosolids-borne trace elements may be released to the environment when biosolids are used as fertilizers in farm land. Trace element leachate concentrations from biosolids are known to be limited by both organic and inorganic sorbent surfaces; this experimental evidence has not been previously verified with geochemical modeling of sorption reactions. In this study, pH-dependent leaching experiments and sorption isotherm experiments were coupled with a multisurface geochemical modeling approach. Biosolids samples were obtained from Toledo and Chicago wastewater treatment plants; their sorbent surfaces were defined and modeled as a combination of organic matter (OM) and Fe-, Al-, and Mn-oxides. The multisurface geochemical modeling approach was partially successful in predicting the pH-dependent leachate concentrations of As, Cd, Cr, Cu, Mo, Ni, and Zn. Both modeled and experimental data indicated that As and Mo in biosolids were bound to Fe- oxides; Cd, Cr, and Cu were bound mainly to OM; and as pH increased the fractions of Cd and Cu bound to Fe- oxides in the biosolids matrix increased. Ni and Zn were distributed between OM and Fe- oxides, and the percentage of each fraction depended on the pH. This study showed that the multisurface geochemical model could be used to generate As (and to a lesser extent Cd) Freundlich isotherm parameters for biosolids. However, the composition and reactivity of solid and dissolved OM was identified as a source of uncertainty in the modeling results. Therefore, more detailed studies focusing on the reactivity of isolated biosolids OM fractions with regard to proton and metal binding are needed to improve the capability of geochemical models to predict the fate of biosolids-borne trace metals in the environment.
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| 3. |
- Baken, S., et al.
(författare)
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Ageing of vanadium in soils and consequences for bioavailability
- 2012
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Ingår i: European Journal of Soil Science. - : Elsevier. - 1351-0754 .- 1365-2389. ; 63:6, s. 839-847
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Tidskriftsartikel (refereegranskat)abstract
- Total vanadium (V) concentrations in soils commonly range from 20 to 120 mg kg-1. Vanadium added directly to soils is more soluble than geogenic V and can be phytotoxic at doses within this range of background concentrations. However, it is unknown how slow sorption reactions change the fate and effect of added V in soils. This study addresses the changes in V solubility, toxicity and bioavailability in soils over time. Four soils were amended with pentavalent V in the form of a soluble vanadate salt, and extractable V concentrations were monitored over 100 days. The toxicity to barley and tomato plants was evaluated in freshly spiked soils and in the corresponding aged soils that were equilibrated for up to 330 days after spiking. The V concentrations in 0.01 m CaCl2 soil extracts decreased approximately two-fold between 14 and 100 days after soil spiking, and the reaction kinetics were similar for all soils. The phytotoxicity of added V decreased on average two-fold between freshly spiked and aged soils. The reduced toxicity was associated with a corresponding decrease in V concentrations in the isolated soil solutions and in the shoots. The V speciation in the soil solution of the aged soils was dominated by V(V); less than 8% was present as V(IV). Oxalate extractions suggest that the V(V) added to soils is predominantly sorbed onto poorly crystalline oxyhydroxides. It is concluded that the toxicity of V measured in freshly spiked soils may not be representative of soils subject to a long-term V contamination in the field.
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| 4. |
- Baken, Stijn, et al.
(författare)
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Characterisation of hydrous ferric oxides derived from iron-rich groundwaters and their contribution to the suspended sediment of streams
- 2013
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Ingår i: Applied Geochemistry. - : Elsevier BV. - 0883-2927 .- 1872-9134. ; 39, s. 59-68
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Tidskriftsartikel (refereegranskat)abstract
- When Fe(II) bearing groundwaters surface in streams, particulate authigenic Fe-rich material is produced by oxidation. Such freshly precipitated Fe minerals may be transported as suspended sediment and have a profound impact on the fate of trace metals and nutrients in rivers. The objective of this study was to monitor changes in mineralogy and composition of authigenic material from its source to streams of increasing order. Groundwaters, surface waters, and suspended sediment in streams of different order were sampled in the Kleine Nete catchment (Belgium), a lowland with Fe-rich groundwaters (3.5-53.8 mg Fe/L; pH 6.3-6.9). Fresh authigenic material (>0.45 mu m) was produced by oxidising filtered (<0.45 mu m) groundwater and surface water. This material contained, on average, 44% Fe, and smaller concentrations of C, P, and Ca. Iron EXAFS (Extended X-ray Absorption Fine Structure) spectroscopy showed that the Fe was present as poorly crystalline hydrous ferric oxides with a structure similar to that of ferrihydrite. The Fe concentration in the suspended sediment samples decreased to 36-40% (stream order 2), and further to 18-26% (stream order 4 and 5). Conversely, the concentrations of organic C, Ca, Si, and trace metals increased with increasing stream order, suggesting mixing of authigenic material with suspended sediment from a different source. The Fe speciation in the suspended sediment was similar to that in fresh authigenic material, but more Fe-Fe interactions were observed, i.e. it was increasingly hydrolysed, suggesting ageing reactions. The suspended sediment in the streams of order 4 and 5 is estimated to contain between 31% and 59% of authigenic material, but more data are needed to refine this estimate. The authigenic material is an important sink for P in these streams which may alleviate the eutrophication risk in this catchment.
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| 5. |
- Baken, Stijn, et al.
(författare)
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The association between iron and carbon in freshwater colloids
- 2013
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Konferensbidrag (refereegranskat)abstract
- Iron and carbon are important constituents of natural colloids, which intimately links the fate of these two elements in riverine systems. Iron may strongly affect the binding of trace metals by organic matter, e.g. through competition for binding sites, which highlights the importance of a correct appreciation of the Fe speciation in surface waters. However, the chemistry of Fe and C in natural colloids is complex and depend on many factors including the pH, the Fe:C ratio, and the redox speciation of Fe [1-3]. Two areas with a contrasting Fe chemistry were studied: a lowland area with widespread seepage of iron-rich groundwater, and an upland peat area. Samples of ten oxic, well-mixed streams were subjected to cascade filtration using conventional filtration (1.2 µm, 0.45 µm, 0.1 µm) and cross-flow ultrafiltration (CFF; 5 kDa). The colloidal fraction, here operationally defined as between 0.45 µm and 5 kDa, was isolated by CFF and subsequently freeze-dried. The speciation of colloidal Fe was determined by EXAFS spectroscopy at the Fe K-edge (MAX-lab, Lund, Sweden). In the rivers draining upland peat, Fe and C were predominantly recovered in the fraction between 5 kDa and 0.1 µm. Conversely, in the rivers draining the lowland with extensive seepage of iron-rich groundwater, Fe was most abundant in the > 0.1 µm fraction, whereas C was predominantly present < 0.1 µm. The EXAFS data reveal that colloidal Fe speciation is different in both study areas. It exists as mononuclear Fe complexed by dissolved organic matter, as colloidal hydrous ferric oxides (likely stabilized by adsorbed organic matter), or as a mixture of these. The colloidal Fe concentrations show considerable seasonal variability. Overall, this study contributes to a better understanding of colloidal Fe speciation and of its interaction with organic C.
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| 6. |
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| 7. |
- Berggren Kleja, Dan, et al.
(författare)
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Characterization of iron in floating surface films of some natural waters using EXAFS
- 2012
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Ingår i: Chemical Geology. - : Elsevier. - 0009-2541 .- 1872-6836. ; 326, s. 19-26
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Tidskriftsartikel (refereegranskat)abstract
- Floating, iron bearing films have been observed in a wide range of environments, including wetlands, seep waters in ground water discharge areas, small rivers and lakes. To date, knowledge about their formation and composition is scarce. We have investigated the form of iron in floating iron-rich films of different origin, including a pond and a brook, as well as seep water pools of a groundwater discharge area. Sampling sites were located in southern (pond, brook) and central (seep pools) Sweden. Synchrotron-based X-ray absorption spectroscopy (EXAFS and XANES) allowed identification of the iron precipitates present in the films, without any pretreatment. The EXAFS data showed that the iron containing phase formed in the floating films varied in composition between the sites investigated. In the films from two ground water discharge areas, characterized by out-flowing iron(II) rich ground water being high in pH and low in DOC, the iron phase was completely dominated by ferrihydrite. In contrast, surface films sampled from the brook and the pond, the iron speciation showed a mixture of iron(III)-organic complexes and iron (hydr)oxide (most likely ferrihydrite). These waters were oxic and contained higher concentration of DOC than the seep water pools in the ground water discharge areas. The position of the pre-edge peak, which is sensitive to the oxidation state of iron, did not indicate occurrence of iron (II) in any of the films. Elemental composition of one film (seep water), suggested that films contained about one third of organic matter. Ferrihydrite is probably present as small particles with humic material sorbed onto surfaces or included in the particles, making the particles sufficiently hydrophobic to not settle without physical disturbance. The films are fragile and break easily down and become suspended upon disturbance. More studies are warranted in order to understand the mechanism of the formation of these fascinating films and their biogeochemical role.
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| 8. |
- Biswas, Ashis, et al.
(författare)
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Estimating the role of competing ions on the arsenic mobilization processes in the aquifers of Bengal Basin by surface complexation modeling
- 2013
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Konferensbidrag (refereegranskat)abstract
- This study investigates the relative roles of the different competing ions on the arsenic (As) mobilization in the sedimentary aquifers of Bengal basin by surface complexation modeling of the temporal varaibility of As in shallow (<50 m) groundwater. Two sets of piezometers (2×5 = 10), installed at the two sites with relatively contrasting dissolved As concentration in groundwater, were monitored bi-weekly for As and other hydrogeochemical parameters over a period of 20 months. The estimation of the standard deviation (SD) for As(III) reflects strong temporal variation (SD ≥10 μg/L) in all the piezometers of two sites over the monitoring period. Particularly, the variation is more prominent in the shallowest part of the aquifer, where the site specific cyclic trends are evident. While, As(V) shows significant temporal variation in the piezometers of high As site only and no specific trend is reflected in the variation.Two different surface complexation models (SCMs), developed for ferrihydrite and goethite have been explored to account for the observed temporal variation in As(III) and As(V) concentrations. The SCM for ferrihydrite has provided the better estimation for both As(III) and As(V) variations.Among the different competing ions, PO43- appears as the major competitor of As(III) and As(V) adsorption onto ferrihydrite and the competition ability decreases in the order PO43- >> Fe(II) > H4SiO4 = HCO3-. It is further revealed that a small decrease in pH significantly increases the concentration of As(III) and decreases the As(V) concentration and vice versa. The present study suggests that the reductive dissolution of Fe oxyhydroxides alone cannot explain the observed high As concentration in groundwater of the sedimentary aquifers. Perhaps, the reductive dissolution of Fe oxyhydroxides followed by competitive sorption reactions with the aquifer sediment is the processes conducive for As enrichment in the groundwater of Bengal basin.
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| 9. |
- Biswas, Ashis, et al.
(författare)
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Role of competing ions in the mobilization of arsenic in groundwater of Bengal Basin : Insight from surface complexation modeling
- 2014
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Ingår i: Water Research. - : Elsevier. - 0043-1354 .- 1879-2448. ; 55, s. 30-39
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Tidskriftsartikel (refereegranskat)abstract
- This study assesses the role of competing ions in the mobilization of arsenic (As) by surface complexation modeling of the temporal variability of As in groundwater. The potential use of two different surface complexation models (SCMs), developed for ferrihydrite and goethite, has been explored to account for the temporal variation of As(III) and As(V) concentration, monitored in shallow groundwater of Bengal Basin over a period of 20 months. The SCM for ferrihydrite appears as the better predictor of the observed variation in both As(III) and As(V) concentrations in the study sites. It is estimated that among the competing ions, PO43- is the major competitor of As(III) and As(V) adsorption onto Fe oxyhydroxide, and the competition ability decreases in the order PO43- >> Fe(II) > H4SiO4 = HCO- (3.) It is further revealed that a small change in pH can also have a significant effect on the mobility of As(III) and As(V) in the aquifers. A decrease in pH increases the concentration of As(III), whereas it decreases the As(V) concentration and vice versa. The present study suggests that the reductive dissolution of Fe oxyhydroxide alone cannot explain the observed high As concentration in groundwater of the Bengal Basin. This study supports the view that the reductive dissolution of Fe oxyhydroxide followed by competitive sorption reactions with the aquifer sediment is the processes responsible for As enrichment in groundwater.
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| 10. |
- Biswas, Ashis, et al.
(författare)
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Surface complexation modeling of temporal variability of arsenic in groundwater : Estimating the role of competing ions in the mobilization processes
- 2013
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Konferensbidrag (refereegranskat)abstract
- This study investigates the relative roles of different competing ions on the mobilization of arsenic (As) by surface complexation modeling of As rich groundwater in the aquifer of Bengal Basin. Two sets of piezometers, installed at different depths of the shallow aquifer (<50 m), have been monitored for As and other relevant hydrogeochemical parameters over a period of 20 months. The potentiality of two different surface complexation models (SCM), developed for ferrihydrite and goethite has been explored to account for the observed temporal variation in As(III) and As(V) concentration in groundwater. The SCM for ferrihydrite appears as the better predictor for the observed variation in both As(III) and As(V) concentration. It is estimated that among the competing ions PO43- is the major competitor of As(III) and As(V) adsorption into Fe oxyhydroxide and competing ability of the ions decreases as PO43- >> Fe(II) > H4SiO4 = HCO3-. The result of sensitivity test indicates that the competition of PO43- with As for the adsorption sites might already reach nearly to the stage of maxima. It is also shown that a slight increase or decrease in pH can have overwhelming effect on the mobility of As(III) and As(V) by changing their concentration oppositely. It appears that only the reductive dissolution of Fe oxyhydroxide cannot explain the observed high As concentration in the groundwater of Bengal Basin. In absence of potential competition for the adsorption sites, As released due to reductive dissolution of Fe oxyhydroxide would have been re-adsorbed into the residual Fe phases. This study suggests that the reductive dissolution of Fe oxyhydroxide followed by competitive ion exchange with the aquifer sediment is the processes conducive for As enrichment in groundwater of the sedimentary aquifers.
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