1. |
- 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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2. |
- 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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3. |
- 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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4. |
- 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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5. |
- Eveborn, David, 1978-
(författare)
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Sustainable phosphorus removal in onsite wastewater treatment
- 2013
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Aquatic eutrophication is a serious environmental problem that occurs all over the world. To protect surface waters (in particular the Baltic Sea), the regulatory pressure on onsite wastewater treatment (OWT) systems have increased in Sweden. Stringent requirements have led to uncertainties regarding the capability of conventional treatment techniques (soil treatment systems (STS)) to remove phosphorus (P), but they have also stimulated the development and introduction of enhanced P treatment techniques. In this thesis the accumulation and mobility of P as well as the chemical P removal mechanisms were studied in soils and reactive filter media. This knowledge was then used in environmental systems analysis. A model based on life cycle assessment (LCA) methodology was developed to evaluate the overall environmental performance of conventional and enhanced P treatment systems under various local conditions. The P accumulation in the studied STS varied (320-870 g m-3) and the accumulated P was rather mobile in some soils. Phosphorus compounds were identified in alkaline reactive filter media (calcium phosphates predominated) by means of X-ray Absorption Near Edge Structure (XANES). In sandy soils from STS aluminium was found to be a key element for P removal, as evidenced by a strong relationship between oxalate-extractable P and Al. The LCA studies indicated that enhanced P treatment systems may be beneficial from an eutrophication and P recycling perspective but causes increased impacts in terms of global warming and acidification. Despite the drawbacks, enhanced P treatment techniques should be considered suitable substitutes to surface water discharge STS under most conditions. This is because the latter systems have such a strong eutrophication impact. On the other hand, under appropriate conditions, STS with groundwater discharge may be advantageous. These systems generally caused low environmental impacts except for the dispersion of P resources.
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6. |
- Gamfeldt, Lars, 1975, et al.
(författare)
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Higher levels of multiple ecosystem services are found in forests with more tree species
- 2013
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 4
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Tidskriftsartikel (refereegranskat)abstract
- Forests are of major importance to human society, contributing several crucial ecosystem services. Biodiversity is suggested to positively influence multiple services but evidence from natural systems at scales relevant to management is scarce. Here, across a scale of 400,000km2, we report that tree species richness in production forests shows positive to positively hump-shaped relationships with multiple ecosystem services. These include production of tree biomass, soil carbon storage, berry production and game production potential. For example, biomass production was approximately 50% greater with five than with one tree species. In addition, we show positive relationships between tree species richness and proxies for other biodiversity components. Importantly, no single tree species was able to promote all services, and some services were negatively correlated to each other. Management of production forests will therefore benefit from considering multiple tree species to sustain the full range of benefits that the society obtains from forests.
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7. |
- Gustafsson, Jon Petter, 1964-, et al.
(författare)
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Chromium (III) and bismuth (III) complexation to organic matter : EXAFS Spectroscopy and equilibrium modeling
- 2013
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Ingår i: Mineralogical magazine. - 0026-461X .- 1471-8022. ; 77:5, s. 1235-
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Tidskriftsartikel (refereegranskat)abstract
- The complexation of chromium(III) and bismuth(III) to organic matter was investigated by batch equilibrations with Suwannee River Fulvic Acid (SRFA) and with mor layer material (Risbergshöjden Oe). In the SRFA systems, 3 mM chromium(III) solutions were equilibrated with 9 g L-1 SRFA and equilibrated at different pH values ranging from 2 to 6. Characterization of the reaction products was made at MAX-Lab, Lund, Sweden, using Cr K-edge EXAFS spectroscopy at 5 989 eV. The spectra were interpreted using both conventional data treatment using EXAFSPAK and with wavelet transform (WT) analysis. The results show that chromium(III) formed monomeric organic complexes with SRFA. There was no evidence of polymerization with the exception of the particulate phase at pH 6, which was attributed to a limited extent of Cr(OH)3 formation.The mor layer material was equilibrated with chromium(III) and bismuth(III) solutions as a function of pH, time and competing ions (iron(III), aluminium(III), copper(II)). Again CrK-edge and Bi L3-edge EXAFS spectroscopy was used, at 5 989 and 13 419 eV. The experiments showed a predominance of monomeric organic complexes for chromium(III). The sorption of chromium(III) was pH-dependent and to some extent found to be influenced by competition from aluminium(III) and copper(II). Chromium(III) complexation was found to be very slow at pH < 4, and equilibration times of three months or longer were required to reach equilibrium under these conditions. Concerning bismuth(III), complexation was quicker and found to be very strong, with more than 94 % bound at pH 1.2 at a high bismuth(III) loading. EXAFS spectroscopy showed that two complexes were involved, one monomeric and one di- or trimeric, with the latter being predominant at higher pH values, although it was present already at pH 1.2. In the organic bismuth(III) complexes, the bismuth(III) octahedron was found to be strongly distorted, which implies strong binding to organic acid functional groups. The complexation of bismuth(III) remained essentially unchanged even in the presence of a potent competitor such as iron(III).The results from the spectroscopic investigation and from the quantitative solution data were used to calibrate new and improved complexation models for the Stockholm Humic (SHM) and the NICA-Donnan models. In the case of the Stockholm Humic Model, both complexes as found by EXAFS spectroscopy were considered explicitly; this ensured the model to predict minimum competition effects in agreement with the laboratory results.
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8. |
- Gustafsson, Jon Petter, 1964-, et al.
(författare)
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Fosfors betydelse för metallers mobilitet i mark
- 2013
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- The aim with this project was to investigate the role of dissolved phosphate for the adsorption of lead(II), copper(II), cadmium(II) and uranium(VI) onto ferrihydrite and to soils. The methods involved batch studies, EXAFS spectroscopy, and equilibrium modelling. Phosphate was found to significantly enhance the adsorption of all investigated metals onto ferrihydrite. Results obtained so far show that the results are consistent with the formation of ternary surface complexes at low pH, but additional research is required to understand the processes in more detail. Similar enhancements were not observed in soil samples to which phosphate is added, and the reasons for this remain to be fully elucidated. In any case, this research shows that the presence of phosphate may restrict the mobility of many trace metals in environments that contain iron(III) (hydr)oxides.
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9. |
- Gustafsson, Jon Petter, 1964-
(författare)
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Soil chemical behaviour of cadmium pigments from paints
- 2013
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- A review focusing on the thermodynamic stability and dissolution rates of Cd-containing sulphides and selenides from paints is presented. In the surface horizon of Swedish agricultural soils, cadmium sulphide, CdS(s), and cadmium selenide, CdSe(s), are shown to be thermodynamically unstable. The presence of electron acceptors such as oxygen gas and iron(III) will lead to gradual dissolution of these compounds. The dissolution rate of Cd-containing sulphides is dependent on the amount of crystalline zinc sulphide in contact with the cadmium, as zinc will be dissolved preferentially from a mixed cadmium zinc sulphide mineral. In the absence of crystalline zinc sulphide, Cd will be dissolved completely after 1-3 years. The presence of crystalline zinc sulphide can extend the life span of CdS to 1-2 decades; however, sewage sludge contains mostly amorphous ZnS that will dissolve more quickly. In conclusion, if a time frame of several decades is applied, it is very likely that Cd from Cd pigments has a similar solubility and bioavailability as an easily soluble Cd salt such as cadmium chloride.
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10. |
- Herrmann, Inga, et al.
(författare)
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Modeling phosphate transport and removal in a compact bed filled with a mineral-based sorbent for domestic wastewater treatment
- 2013
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Ingår i: Journal of Contaminant Hydrology. - : Elsevier BV. - 0169-7722 .- 1873-6009. ; 154, s. 70-77
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Tidskriftsartikel (refereegranskat)abstract
- Phosphorus filter units containing mineral-based sorbents with a high phosphate (PO4) binding capacity have been shown to be appropriate for removing PO4 in the treatment of domestic wastewater in on-site facilities. However, a better understanding of their PO4 removal mechanisms, and reactions that could lead to the formation of PO4 compounds, is required to evaluate the potential utility of candidate sorbents. Models based on data obtained from laboratory-scale experiments with columns of selected materials can be valuable for acquiring such understanding. Thus, in this study the transport and removal of PO4 in experiments with a laboratory-scale column filled with a commercial silicate-based sorbent were modeled, using the hydro-geochemical transport code PHREEQC. The resulting models, that incorporated the dissolution of calcite, kinetic constrains for the dissolution of calcium oxide (CaO) and wollastonite (CaSiO3), and the precipitation of amorphous tricalcium phosphate, Ca3(PO 4)2, successfully simulated the removal of PO4 observed in the experiments.
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