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- Adediran, Gbotemi A., et al.
(author)
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Phosphorus in 2D : Spatially resolved P speciation in two Swedish forest soils as influenced by apatite weathering and podzolization
- 2020
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In: Geoderma. - : Elsevier BV. - 0016-7061 .- 1872-6259. ; 376
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Journal article (peer-reviewed)abstract
- The cycling and long-term supply of phosphorus (P) in soils are of global environmental and agricultural concern. To advance the knowledge, a detailed understanding of both the vertical and lateral variation of P chemical speciation and retention mechanism(s) is required, a knowledge that is limited in postglacial forest soils. We combined the use of synchrotron X-ray fluorescence microscopy with multi-elemental co-localisation analysis and P K-edge XANES spectroscopy to reveal critical chemical and structural soil properties. We established a two-dimensional (2D) imagery of P retention and speciation at a microscale spatial resolution in two forest soil profiles formed in glaciofluvial and wave-washed sand. The abundance and speciation of P in the upper 40 cm was found to be influenced by soil weathering and podzolization, leading to spatial variability in P speciation on the microscale (< 200 pm) with P existing predominantly as organic P and as PO4 adsorbed to allophane and ferrihydrite, according to XANES spectroscopy. These species were mostly retained at sharp edges and in pore spaces within Al and Si-bearing particles. Despite the relatively young age ( < 15,000 years) of the soils, our results show primary mineral apatite to have weathered from the surface horizons. In the C horizon however, a large fraction of the P was in the form of apatite, which appeared as widely dispersed ( > 600 pm) hot spots of inclusions in aluminosilicates or as discrete micro-sized apatite grains. The subsoil apatite represents a pool of P that trees can potentially acquire and thus add to the biogeochemically active P pool in temperate forest soils.
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3. |
- Adediran, Gbotemi, et al.
(author)
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Micro and nano sized particles in leachates from agricultural soils: Phosphorus and sulfur speciation by X-ray micro-spectroscopy
- 2021
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In: Water Research. - : Elsevier BV. - 0043-1354 .- 1879-2448. ; 189
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Journal article (peer-reviewed)abstract
- Colloids and nanoparticles leached from agricultural land are major carriers of potentially bioavailable nutrients with high mobility in the environment. Despite significant research efforts, accurate knowledge of macronutrients in colloids and nanoparticles is limited. We used multi-elemental synchrotron X-ray fluorescence (XRF) microscopy with multivariate spatial analysis and X-ray atomic absorption near-edge structure (XANES) spectroscopy at the P and S K-edges, to study the speciation of P and S in two fractions of leached particles, >0.45 and <0.45 mu m respectively, collected from four tile-drained agricultural sites in Sweden. P K-edge XANES showed that organic P, followed by P adsorbed to surfaces of aluminum-bearing particles were the most common forms of leached P. Iron-bound P (Fe-P) forms were generally less abundant (0-30 % of the total P). S K-edge XANES showed that S was predominantly organic, and a relatively high abundance of reduced S species suggests that redox conditions were adverse to the persistence of P bound to Fe-bearing colloids in the leachates. Acid ammonium-oxalate extractions suggested that P associated with Al and Fe (Al-P and Fe-P) in most cases could be explained by the adsorption capacity of non-crystalline (oxalate-extractable) oxides of Al and Fe. These results improve our understanding of particulate P and S speciation in the vadose zone and helps in developing effective technologies for mitigating colloidal driven eutrophication of water bodies near agricultural land. (C) 2020 The Author(s). Published by Elsevier Ltd.
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- Aullón Alcaine, Anna, et al.
(author)
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Hydrogeochemical controls on the mobility of arsenic, fluoride and other geogenic co-contaminants in the shallow aquifers of northeastern La Pampa Province in Argentina
- 2020
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In: Science of the Total Environment. - : Elsevier. - 0048-9697 .- 1879-1026. ; 715
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Journal article (peer-reviewed)abstract
- Elevated Arsenic (As) and Fluoride (F) concentrations in groundwater have been studied in the shallow aquifers of northeastern of La Pampa province, in the Chaco-Pampean plain, Argentina. The source of As and co-contaminants is mainly geogenic, from the weathering of volcanic ash and loess (rhyolitic glass) that erupted from the Andean volcanic range. In this study we have assessed the groundwater quality in two semi-arid areas of La Pampa. We have also identified the spatial distribution of As and co-contaminants in groundwater and determined the major factors controlling the mobilization of As in the shallow aquifers. The groundwater samples were circum-neutral to alkaline (7.4 to 92), oxidizing (Eh similar to 0.24 V) and characterized by high salinity (EC = 456-11,400 mu S/cm) and Na+-HCO3- water types in recharge areas. Carbonate concretions ("tosca") were abundant in the upper layers of the shallow aquifer. The concentration of total As (5.6 to 535 mu g/L) and F (0.5 to 14.2 mg/L) were heterogeneous and exceeded the recommended WHO Guidelines and the Argentine Standards for drinking water. The predominant As species were arsenate As(V) oxyanions, determined by thermodynamic calculations. Arsenic was positively correlated with bicarbonate (HCO3-), fluoride (F), boron (B) and vanadium (V), but negatively correlated with iron (Fe), aluminium (Al), and manganese (Mn), which were present in low concentrations. The highest amount of As in sediments was from the surface of the dry lake. The mechanisms for As mobilization are associated with multiple factors: geochemical reactions, hydrogeological characteristics of the local aquifer and climatic factors. Desorption of As(V) at high pH, and ion competition for adsorption sites are considered the principal mechanisms for As mobilization in the shallow aquifers. In addition, the long-term consumption of the groundwater could pose a threat for the health of the local community and low cost remediation techniques are required to improve the drinking water quality.
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5. |
- Berggren Kleja, Dan, et al.
(author)
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Bismuth(III) Forms Exceptionally Strong Complexes with Natural Organic Matter
- 2022
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56, s. 3076-3084
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Journal article (peer-reviewed)abstract
- The use of bismuth in the society has steadily increased during the last decades, both as a substitute for lead in hunting ammunition and various metallurgical applications, as well as in a range of consumer products. At the same time, the environmental behavior of bismuth is largely unknown. Here, the binding of bismuth(III) to organic soil material was investigated using extended X-ray absorption spectroscopy (EXAFS) and batch experiments. Moreover, the capacity of suwannee river fulvic acid (SRFA) to enhance the solubility of metallic bismuth was studied in a long-term (2 years) equilibration experiment. Bismuth(III) formed exceptionally strong complexes with the organic soil material, where >99% of the added bismuth(III) was bound by the solid phase, even at pH 1.2. EXAFS data suggest that bismuth(III) was bound to soil organic matter as a dimeric Bi3+ complex where one carboxylate bridges two Bi3+ ions, resulting in a unique structural stability. The strong binding to natural organic matter was verified for SRFA, dissolving 16.5 mmol Bi per gram carbon, which largely exceeds the carboxylic acid group density of this compound. Our study shows that bismuth(III) will most likely be associated with natural organic matter in soils, sediments, and waters.
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- Braun, Sabina, et al.
(author)
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Phosphorus desorption and isotope exchange kinetics in agricultural soils
- 2020
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In: Soil use and management. - : Wiley. - 0266-0032 .- 1475-2743.
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Journal article (peer-reviewed)abstract
- To improve phosphorus (P) fertilization and environmental assessments, a better understanding of release kinetics of solid-phase P to soil solution is needed. In this study, Fe (hydr)oxide-coated filter papers (Fh papers), isotopic exchange kinetics (IEK) and chemical extractions were used to assess the sizes of fast and slowly desorbing P pools in the soils of six long-term Swedish field experiments. The P desorption data from the Fh-paper extraction of soil (20 days of continual P removal) were fitted with the Lookman two-compartment desorption model, which estimates the pools of fast (Q1) and slowly (Q2) desorbing P, and their desorption rates k1 and k2. The amounts of isotope-exchangeable P (E) were calculated (E1min to E>3 months) and compared with Q1 and Q2. The strongest relationship was found between E1 min and Q1 (r2 =.87, p <.01). There was also an inverse relationship between the IEK parameter n (the rate of exchange) and k1 (r2 =.52, p <.01) and k2 (r2 =.52, p <.01), suggesting that a soil with a high value of n desorbs less P per time unit. The relationships between these results show that they deliver similar information, but both methods are hard to implement in routine analysis. However, Olsen-extractable P was similar in magnitude to Q1 (P-Olsen = 1.1 × Q1 + 2.3, r2 =.96), n and k1 were related to P-Olsen/P-CaCl2, while k2 was related to P-oxalate/P-Olsen. Therefore, these extractions can be used to estimate the sizes and desorption rates of the different P pools, which could be important for assessments of plant availability and leaching.
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- Campos-Pereira, Hugo, et al.
(author)
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Effect of pH, surface charge and soil properties on the solid-solution partitioning of perfluoroalkyl substances (PFASs) in a wide range of temperate soils
- 2023
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In: Chemosphere. - : PERGAMON-ELSEVIER SCIENCE LTD. - 0045-6535 .- 1879-1298. ; 321
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Journal article (peer-reviewed)abstract
- The pH-dependent soil-water partitioning of six perfluoroalkyl substances (PFASs) of environmental concern (PFOA, PFDA, PFUnDA, PFHxS, PFOS and FOSA), was investigated for 11 temperate mineral soils and related to soil properties such as organic carbon content (0.2-3%), concentrations of Fe and Al (hydr)oxides, and texture. PFAS sorption was positively related to the perfluorocarbon chain length of the molecule, and inversely related to solution pH for all substances. The negative slope between log Kd and pH became steeper with increasing perfluorocarbon chain length of the PFAS (r2 = 0.75, p <= 0.05). Organic carbon (OC) alone was a poor predictor of the partitioning for all PFASs, except for FOSA (r2 = 0.71), and the OC-normalized PFAS partitioning, as derived from organic soil materials, underestimated PFAS sorption to the soils. Multiple linear regression suggested sorption contributions (p <= 0.05) from OC for perfluorooctane sulfonate (PFOS) and FOSA, and Fe/Al (hydr) oxides for PFOS, FOSA, and perfluorodecanoate (PFDA). FOSA was the only substance under study for which there was a statistically significant correlation between its binding and soil texture (silt + clay). To predict PFAS sorption, the surface net charge of the soil organic matter fraction of all soils was calculated using the Stockholm Humic Model. When calibrated against charge-dependent PFAS sorption to a peat (Oe) material, the derived model significantly underestimated the measured Kd values for 10 out of 11 soils. To conclude, additional
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8. |
- de Campos Pereira, Hugo, et al.
(author)
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Binding of per- and polyfluoroalkyl substances (PFASs) by organic soil materials with different structural composition - Charge- and concentration-dependent sorption behavior
- 2022
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In: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 297
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Journal article (peer-reviewed)abstract
- The charge-and concentration-dependent sorption behavior of a range of per-and polyfluoroalkyl substances (PFASs) was studied for three organic soil samples with different organic matter quality, one Spodosol Oe horizon (Mor Oe) and two Sphagnum peats with different degrees of decomposition (Peat Oi and Peat Oe). Sorption to the two peat materials was, on average, four times stronger compared to that onto the Mor Oe material. In particular, longer-chained PFASs were more strongly bound by the two peats as compared to the Mor Oe sample. The combined results of batch sorption experiments and 13C NMR spectroscopy suggested sorption to be positively related to the content of carbohydrates (i.e., O-alkyl carbon). Sorption of all PFAS subclasses was inversely related to the pH value in all soils, with the largest pH effects being observed for perfluoroalkyl carboxylates (PFCAs) with C-10 and C-11 perfluorocarbon chain lengths. Experimentally determined sorption isotherms onto the poorly humified Peat Oi did not deviate significantly from linearity for most substances, while for the Mor Oe horizon, sorption nonlinearity was generally more pronounced. This work should prove useful in assessing PFAS sorption and leaching in organic soil horizons within environmental risk assessment.
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9. |
- de Campos Pereira, Hugo, et al.
(author)
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The Adsorption of Per- and Polyfluoroalkyl Substances (PFASs) onto Ferrihydrite Is Governed by Surface Charge
- 2020
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 54, s. 15722-15730
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Journal article (peer-reviewed)abstract
- An improved quantitative and qualitative understanding of the interaction of per- and polyfluoroalkyl substances (PFASs) and short-range ordered Fe (hydr)oxides is crucial for environmental risk assessment in environments low in natural organic matter. Here, we present data on the pH-dependent sorption behavior of 12 PFASs onto ferrihydrite. The nature of the binding mechanisms was investigated by sulfur K-edge X-ray absorption near-edge structure (XANES) spectroscopy and by phosphate competition experiments. Sulfur K-edge XANES spectroscopy showed that the sulfur atom of the head group of the sulfonated PFASs retained an oxidation state of +V after adsorption. Furthermore, the XANES spectra did not indicate any involvement of inner-sphere surface complexes in the sorption process. Adsorption was inversely related to pH (p < 0.05) for all PFASs (i.e., C-3-C-5 and C-7-C-9 perfluorocarboxylates, C-4, C-6, and C-8 perfluorosulfonates, perfluorooctane sulfonamide, and 6:2 and 8:2 fluorotelomer sulfonates). This was attributed to the pH-dependent charge of the ferrihydrite surface, as reflected in the decrease of surface zeta-potential with increasing pH. The importance of surface charge for PFAS adsorption was further corroborated by the observation that the adsorption of PFASs decreased upon phosphate adsorption in a way that was consistent with the decrease in ferrihydrite zeta-potential. The results show that ferrihydrite can be an important sorbent for PFASs with six or more perfluorinated carbons in acid environments (pH <= 5), particularly when phosphate and other competitors are present in relatively low concentrations.
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10. |
- Envall, Ida, et al.
(author)
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Existing evidence related to soil retention of phosphorus from on-site wastewater treatment systems in boreal and temperate climate zones : a systematic map
- 2023
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In: Environmental Evidence. - : Springer Nature. - 2047-2382. ; 12:1
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Journal article (peer-reviewed)abstract
- Background: In Sweden there are nearly one million soil-based on-site wastewater treatment systems (OWTSs). OWTSs may contribute to eutrophication of surface waters, due to the discharge of phosphorus (P). Hence, in certain cases, a high P removal rate (up to 90%) of OWTSs is required by Swedish authorities. Since these requirements may have costly consequences to property owners, it is debated whether they are too strict. In this debate, it is often claimed that the soil retention of P occurring in the natural environments may be underestimated by authorities. Soil retention is the inhibition of the transport of P through the ground, due to different chemical, physical and biological processes occurring there. These processes make the P transport slower, which may reduce the unwanted impact on receiving water bodies. However, the efficiency of soil retention of P remains unclear. The objective of this systematic map was to collect, code, organise and elucidate the relevant evidence related to the topic, to be able to guide stakeholders through the evidence base, and to support future research synthesising, commissioning, and funding. The systematic map was carried out in response to needs declared by the Swedish Agency for Marine and Water Management but the conclusions should be valid for a wider range of countries across boreo-temperate regions.Methods: Searches were made for peer-reviewed and grey literature using bibliographic databases, search engines, specialist websites, and stakeholder contacts. The references were screened for relevance according to a predefined set of eligibility criteria. A detailed database of the relevant studies was compiled. Data and metadata that enable evaluation and discussion of the character and quality of the evidence base were extracted and coded. Special focus was placed on assessing if existing evidence could contribute to policy and practice decision making. Descriptive information about the evidence base was presented in tables and figures. An interactive evidence atlas and a choropleth were created, displaying the locations of all studies.Review findings: 234 articles out of 10,797 screened records fulfilled the eligibility criteria. These articles contain 256 studies, performed in the field or in the laboratory. Six different study types were identified, based on where the measurements were conducted. Most studies, including laboratory studies, lack replicates. Most field studies are observational case studies.Conclusions: It is not possible to derive valid generic measures of the efficiency of soil retention of P occurring in the natural soil environment from available research. Neither does the evidence base allow for answering the question of the magnitude of the potential impact of OWTSs on the P concentration in recipients on a general basis, or under what conditions OWTSs generally have such an impact. A compilation of groundwater studies may provide examples of how far the P may reach in x years, but the number of groundwater studies is insufficient to draw any general conclusions, given the complexity and variability of the systems. Future research should strive for replicated study designs, more elaborate reporting, and the establishment of a reporting standard.
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