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Yu, C., Berger, T., Drake, H., Song, Z., Peltola, P. & Åström, M. E. (2019). Geochemical controls on dispersion of U and Th in Quaternary deposits, stream water, and aquatic plants in an area with a granite pluton. Science of the Total Environment, 663, 16-28
Open this publication in new window or tab >>Geochemical controls on dispersion of U and Th in Quaternary deposits, stream water, and aquatic plants in an area with a granite pluton
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2019 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 663, p. 16-28Article in journal (Refereed) Published
Abstract [en]

The weathering of U and/or Th rich granite plutons, which occurs worldwide, may serve as a potentially important, but as yet poorly defined source for U and Th in (sub-)surface environments. Here, we assessed the impact of an outcrop of such granite (5 km in diameter) and its erosional products on the distribution of U and Th in four nemo-boreal catchments. The results showed that (i) the pluton was enriched in both U and Th; and (ii) secondary U and Th phases were accumulated by peat/gyttja and in other Quaternary deposits with high contents of organic matter. Movement of the ice sheet during the latest glaciation led to dispersal of U- and Th-rich materials eroded from the pluton, resulting in a progressive increase in dissolved U and Th concentrations, as well as U concentrations in aquatic plants with increasing proximity to the pluton. The accumulation of U in the aquatic plants growing upon the pluton (100–365 mg kg−1, dry ash weight) shows that this rock represents a long-term risk for adjacent ecosystems. Dissolved pools of U and Th were correlated with those of dissolved organic matter (DOM) and were predicted to largely occur as organic complexes. This demonstrates the importance of DOM in the transport of U and Th in the catchments. Large fractions of Ca2UO2(CO3)30(aq) were modeled to occur in the stream with highest pH and alkalinity and thus, explain the strongly elevated U concentrations and fluxes in this particular stream. In future climate scenarios, boreal catchments will experience intensified runoff and warmer temperature that favor the production of hydrologically accessible DOM and alkalinity. Therefore, the results obtained from this study have implications for predicting the distribution and transport of Th and U in boreal catchments, especially those associated with U and/or Th rich granite plutons.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Uranium, Thorium, Nemo-boreal catchments, Climate change, Weathering
National Category
Environmental Sciences Geochemistry
Research subject
Natural Science, Environmental Science; Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-80032 (URN)10.1016/j.scitotenv.2019.01.293 (DOI)000459858500002 ()30708213 (PubMedID)
Available from: 2019-01-30 Created: 2019-01-30 Last updated: 2019-03-15Bibliographically approved
Yang, S., Hao, Q., Liu, H., Xiaodong, Z., Yu, C., Yang, X., . . . Song, Z. (2019). Impact of grassland degradation on the distribution and bioavailability of soil silicon: Implications for the Si cycle in grasslands [Letter to the editor]. Science of the Total Environment, 657, 811-818
Open this publication in new window or tab >>Impact of grassland degradation on the distribution and bioavailability of soil silicon: Implications for the Si cycle in grasslands
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2019 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 657, p. 811-818Article in journal, Letter (Refereed) Published
Abstract [en]

Grassland ecosystems play an important role in the global terrestrial silicon (Si) cycle, and Si is a beneficial elementand structural constituent for the growth of grasses. In previous decades, grasslands have been degradedto different degrees because of the drying climate and intense human disturbance. However, the impact of grasslanddegradation on the distribution and bioavailability of soil Si is largely unknown. Here, we investigated vegetationand soil conditions of 30 sites to characterize different degrees of degradation for grasslands in the agropastoralecotone of northern China. We then explored the impact of grassland degradation on the distributionand bioavailability of soil Si, including total Si and four forms of noncrystalline Si in three horizons (0–10,10–20 and 20–40 cm) of different soil profiles. The concentrations of noncrystalline Si in soil profiles significantlydecreased with increasing degrees of degradation, being 7.35 ± 0.88 mg g−1, 5.36 ± 0.39 mg g−1, 3.81 ±0.37 mg g−1 and 3.60±0.26 mg g−1 in non-degraded, lightly degraded, moderately degraded and seriously degradedgrasslands, respectively. Moreover, the storage of noncrystalline Si decreased from higher than 40 t ha−1to lower than 23 t ha−1. The corresponding bioavailability of soil Si also generally decreased with grassland degradation.These processes may not only affect the Si pools and fluxes in soils but also influence the Si uptake in 

plants. We suggest that grassland degradation can significantly affect the global grassland Si cycle. Grasslandmanagement methods such as fertilizing and avoiding overgrazing can potentially double the content and storageof noncrystalline Si in soils, thereby enhancing the soil Si bioavailability by N17%.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Silicon cycle, Bioavailability, Grassland degradation, Agro-pastoral ecotone, Northern China
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science; Natural Science
Identifiers
urn:nbn:se:lnu:diva-79201 (URN)10.1016/j.scitotenv.2018.12.101 (DOI)000455903400079 ()30677946 (PubMedID)
Available from: 2018-12-13 Created: 2018-12-13 Last updated: 2019-02-05Bibliographically approved
Yu, C., Drake, H., Lopez-Fernandez, M., Whitehouse, M., Dopson, M. & Åström, M. E. (2019). Micro-scale isotopic variability of low-temperature pyrite in fractured crystalline bedrock ― A large Fe isotope fractionation between Fe(II)aq/pyrite and absence of Fe-S isotope co-variation [Letter to the editor]. Chemical Geology, 522, 192-207
Open this publication in new window or tab >>Micro-scale isotopic variability of low-temperature pyrite in fractured crystalline bedrock ― A large Fe isotope fractionation between Fe(II)aq/pyrite and absence of Fe-S isotope co-variation
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2019 (English)In: Chemical Geology, ISSN 0009-2541, E-ISSN 1872-6836, Vol. 522, p. 192-207Article in journal, Letter (Refereed) In press
Abstract [en]

This study assessed Fe-isotope ratio (56Fe/54Fe, expressed as δ56Fe relative to the IRMM-014 standard) variability and controls in pyrite that has among the largest reported S-isotope variability (maximum δ34S: 140‰). The pyrite occurs as fine-grained secondary crystals in fractures throughout the upper kilometer of granitoids of the Baltic Shield, and was analyzed here for δ56Fe by in situ secondary ion mass spectrometry (SIMS). Part of these pyrite crystals were picked from borehole instrumentation at depths of >400 m below sea level (m.b.s.l.), and thus are modern (known to have formed within 17 years) and can be compared with the δ56Fe of the source dissolved ferrous iron. The δ56Fe values of the modern pyrite crystals (−1.81‰ to +2.29‰) varied to a much greater extent than those of the groundwaters from which they formed (−0.48‰ to +0.13‰), providing strong field evidence for a large Fe isotope fractionation during the conversion of Fe(II)aq to FeS and ultimately to pyrite. Enrichment of 56Fe in pyrite relative to the groundwater was explained by equilibrium Fe(II)aq-FeS isotope fractionation, whereas depletion of 56Fe in pyrite relative to the groundwater was mainly the result of sulfidization of magnetite and kinetic isotopic fractionation during partial transformation of microsized FeS to pyrite. In many pyrite crystals, there is an increase in δ34S from crystal center to rim reflecting Rayleigh distillation processes (reservoir effects) caused by the development of closed-system conditions in the micro-environment near the growing crystals. A corresponding center-to-rim feature was not observed for the δ56Fe values. It is therefore unlikely that the groundwater near the growing pyrite crystals became progressively enriched in the heavy Fe isotope, in contrast to what has been found for the sulfur in sulfate. Other pyrite crystals formed following bacterial sulfate reduction in the time period of mid-Mesozoicum to Quaternary, had an almost identical Fe-isotope variability (total range: −1.50‰ to +2.76‰), frequency-distribution pattern, and relationship with δ34S as the recent pyrite formed on the borehole instrumentation. These features suggest that fundamental processes are operating and governing the Fe-isotope composition of pyrite crystals formed in fractured crystalline bedrock over large time scales.

Keywords
Pyrite, Iron isotopes, Equilibrium Fe-isotope fractionation, Magnetite sulfidization, Partial pyritization, Fractured crystalline bedrock
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-84618 (URN)10.1016/j.chemgeo.2019.05.026 (DOI)
Available from: 2019-06-05 Created: 2019-06-05 Last updated: 2019-06-05
Yu, C., Boily, J.-F., Shchukarev, A., Drake, H., Song, Z., Hogmalm, K. J. & Åström, M. E. (2018). A cryogenic XPS study of Ce fixation on nanosized manganite and vernadite: Interfacial reactions and effects of fulvic acid complexation. Chemical Geology, 483, 304-311
Open this publication in new window or tab >>A cryogenic XPS study of Ce fixation on nanosized manganite and vernadite: Interfacial reactions and effects of fulvic acid complexation
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2018 (English)In: Chemical Geology, ISSN 0009-2541, E-ISSN 1872-6836, Vol. 483, p. 304-311Article in journal (Refereed) Published
Abstract [en]

This study investigated interfacial reactions between aqueous Ce(III) and two synthetic nanosized Mn (hydr-) oxides (manganite: γ-MnOOH, and vernadite: δ-MnO2) in the absence and presence of Nordic Lake fulvic acid (NLFA) at circumneutral pH by batch experiments and cryogenic X-ray photoelectron spectroscopy (XPS). The surfaces of manganite and vernadite were negatively charged (XPS-derived loadings of (Na+K)/Cl > 1) and loaded with 0.42–4.33 Ce ions nm−2. Manganite stabilized Ce-oxidation states almost identical to those for vernadite (approximately 75% Ce(IV) and 25% Ce(III)), providing the first experimental evidence that also a Mn (III) phase (manganite) can act as an important scavenger for Ce(IV) and thus, contribute to the decoupling of Ce from its neighboring rare earth elements and the development of Ce anomaly. In contrast, when exposed to Ce (III)-NLFA complexes, the oxidation of Ce by these two Mn (hydr-)oxides was strongly suppressed, suggesting that the formation of Ce(III) complexes with fulvic acid can stabilize Ce(III) even in the presence of oxidative Mn oxide surfaces. The experiments also showed that Ce(III) complexed with excess NLFA was nearly completely removed, pointing to a strong preferential sorption of Ce(III)-complexed NLFA over free NLFA. This finding suggests that the Ce(III)-NLFA complexes were most likely sorbed by their cation side, i.e. Ce(III) bridging between oxide groups on the Mn (hydr-)oxides and negatively-charged functional groups in NLFA. Hence, Ce(III) was in direct contact with the oxidative manganite and vernadite but despite that not oxidized. An implication is that in organic-rich environments there may be an absence of Ce(IV) and Ce anomaly despite otherwise favorable conditions for Ce(III) oxidation.

Place, publisher, year, edition, pages
Elsevier, 2018
Keywords
Cryogenic XPS, Manganite, Vernadite, Oxidative scavenging, Ce anomaly
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science
Identifiers
urn:nbn:se:lnu:diva-72684 (URN)10.1016/j.chemgeo.2018.02.033 (DOI)000429492300027 ()
Available from: 2018-04-13 Created: 2018-04-13 Last updated: 2018-07-10Bibliographically approved
Li, Z., Song, Z., Yang, X., Song, A., Yu, C., Wang, T., . . . Liang, Y. (2018). Impacts of silicon on biogeochemical cycles of carbon and nutrients in croplands. Journal of Integrative Agriculture, 17(10), 2182-2195
Open this publication in new window or tab >>Impacts of silicon on biogeochemical cycles of carbon and nutrients in croplands
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2018 (English)In: Journal of Integrative Agriculture, ISSN 2095-3119, Vol. 17, no 10, p. 2182-2195Article, review/survey (Refereed) Published
Abstract [en]

Crop harvesting and residue removal from croplands often result in imbalanced biogeochemical cycles of carbon and nutrients in croplands, putting forward an austere challenge to sustainable agricultural production. As a beneficial element, silicon(Si) has multiple eco-physiological functions, which could help crops to acclimatize their unfavorable habitats. Although many studies have reported that the application of Si can alleviate multiple abiotic and biotic stresses and increase biomass accumulation, the effects of Si on carbon immobilization and nutrients uptake into plants in croplands have not yet been explored. This review focused on Si-associated regulation of plant carbon accumulation, lignin biosynthesis, and nutrients uptake, which are important for biogeochemical cycles of carbon and nutrients in croplands. The tradeoff analysis   the supply of bioavailable Si can enhance plant net photosynthetic rate and biomass carbon production (especially root biomass input to soil organic carbon pool), but reduce shoot lignin biosynthesis. Besides, the application of Si could improve uptake of most nutrients under deficient conditions, but restricts excess uptake when they are supplied in surplus amounts. Nevertheless, Si application to crops may enhance the uptake of nitrogen and iron when they are supplied in deficient to luxurious amounts, while potassium uptake enhanced by Si application is often involved in alleviating salt stress and inhibiting excess sodium uptake in plants. More importantly, the amount of Si accumulated in plant positively correlates with nutrients release during the decay of crop biomass, but negatively correlates with straw decomposability due to the reduced lignin synthesis. The Si-mediated plant growth and litter decomposition collectively suggest that Si cycling in croplands plays important roles in biogeochemical cycles of carbon and nutrients. Hence, scientific Si management in croplands will be helpful for maintaining sustainable development of agriculture.

Place, publisher, year, edition, pages
Elsevier, 2018
Keywords
silicon, cropland, biogeochemical cycle, biomass carbon, nutrient
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-78089 (URN)10.1016/S2095-3119(18)62018-0 (DOI)000446519800006 ()
Available from: 2018-09-30 Created: 2018-09-30 Last updated: 2018-10-24Bibliographically approved
Åström, M. E., Yu, C., Peltola, P., Reynolds, J. K., Österholm, P., Nystrand, M. I., . . . Ojala, A. E. .. (2018). Sources, transport and sinks of beryllium in a coastal landscape affected by acidic soils. Geochimica et Cosmochimica Acta, 232, 288-302
Open this publication in new window or tab >>Sources, transport and sinks of beryllium in a coastal landscape affected by acidic soils
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2018 (English)In: Geochimica et Cosmochimica Acta, ISSN 0016-7037, E-ISSN 1872-9533, Vol. 232, p. 288-302Article in journal (Refereed) Published
Abstract [en]

Beryllium (Be) sources, transport and sinks were studied in a coastal landscape where acidic soils (acid sulfate soils) have developed after drainage of fine-grained sulfide-bearing sediments. The study included the determination of total abundance and speciation of Be in a variety of solid and aqueous materials in both the terrestrial and estuarine parts of the landscape. A major feature was that despite normal (background) Be concentration in the sulfide-bearing sediments, the Be leaching from these sediments after O2-exposure and acid sulfate soil development were extensive, with concentrations up to 76 μg L−1 in soil water, 39 μg L−1 in runoff and 12 μg L−1 in low-order streams. These high Be concentrations were mainly in the solution form (i.e., passing a 1 kilodalton filter) and modelled to be dominated by free Be2+. The extensive Be release within, and leaching from the acid sulfate soils was controlled by pH, with a critical value of 4.0 below which the Be concentrations increased strongly. Although plagioclase and mica were most likely the main carriers of Be within these soils, it is suggested that other minerals such as Be hydroxides, Al hydroxides carrying Be, and Be sulfides are the main contributors of the abundance of dissolved Be in the acidic waters. When the acidic and Be-rich creek water was neutralized in the estuary of relatively low salinity, the dominating solution form of Be was removed by transformation to particles, reflected in the suspended particulate matter that had hydroxylamine hydrochloride extractable Be up to 17 mg kg−1 and ammonium acetate EDTA extractable Be up to 4 mg kg−1. In corresponding pristine materials (parent material of the acid sulfate soils) in the catchment, the median Be extractability with these reagents were only 0.3 and 0.05 mg kg−1, respectively. As the Be-rich suspended particulate matter ultimately became benthic sediment, the Be was preserved in terms of total concentrations but underwent to some extent changes in speciation, including release from hydroxides and concomitant scavenging by organic matter and particle surfaces.

Place, publisher, year, edition, pages
Elsevier, 2018
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-74838 (URN)10.1016/j.gca.2018.04.025 (DOI)000432751700015 ()
Available from: 2018-06-01 Created: 2018-06-01 Last updated: 2019-05-24Bibliographically approved
Yu, C., Drake, H., Mathurin, F. A. & Åström, M. E. (2017). Cerium sequestration and accumulation in fractured crystalline bedrock: The role of Mn-Fe (hydr-)oxides and clay minerals. Geochimica et Cosmochimica Acta, 199, 370-389
Open this publication in new window or tab >>Cerium sequestration and accumulation in fractured crystalline bedrock: The role of Mn-Fe (hydr-)oxides and clay minerals
2017 (English)In: Geochimica et Cosmochimica Acta, ISSN 0016-7037, E-ISSN 1872-9533, Vol. 199, p. 370-389Article in journal (Refereed) Published
Abstract [en]

This study focuses on the mechanisms of Ce sequestration and accumulation in the fracture network of the upper kilometer of the granitoid bedrock of the Baltic Shield in southeast Sweden (Laxemar area, Sweden). The material includes 81 specimens of bulk secondary mineral precipitates ("fracture coatings") collected on fracture walls identified in 17 drill cores, and 66 groundwater samples collected from 21 deep boreholes with equipment designed for retrieval of representative groundwater at controlled depths. The concentrations of Ce in the fracture coatings, although varying considerably (10-90th percentiles: 67-438 mg kg(-1)), were frequently higher than those of the wall rock (10-90th percentiles: 70-118 mg kg(-1)). Linear combination fitting analysis of Ce L-III-edge X-ray absorption near-edge structure (XANES) spectra, obtained for 19 fracture coatings with relatively high Ce concentrations (>= 145 mg kg(-1)) and a wide range of Ce-anomaly values, revealed that Ce(IV) occurs frequently in the upper 10 m of the fracture network (Ce(IV)/Ce-total = 0.06-1.00 in 8 out of 11 specimens) and is mainly associated with Mn oxides (modeled as Ce oxidatively scavenged by birnessite). These features are in line with the strong oxidative and sorptive capacities of Mn oxide as demonstrated by previous studies, and abundant todorokite and birnessite-like Mn oxides identified in 3 out of 4 specimens analyzed by Mn K-edge X-ray absorption spectroscopy (XAS) in the upper parts of the fracture network (down to 5 m). For a specimen with very high Ce concentration (1430 mg kg(-1)) and NASC-normalized Ce anomaly (3.63), the analysis of Ce XANES and Mn XAS data revealed (i) a predominance of Ce oxide in addition to Ce scavenged by Mn oxide; and (ii) a large fraction of poorly-crystalline hexagonal birnessite and aqueous Mn2+, suggesting a recent or on-going oxidation of Mn2+ in this fracture. In addition, the Ce oxide precipitates on this fracture observed by in situ SEM-EDS contained considerable amounts of Mn. These spectroscopic and microscopic features led us to suggest that the remarkable accumulation of Ce(IV) in this fracture is a result of repeated formation and dissolution of Mn oxides, that is, formation of Mn oxide followed by oxidative scavenging of Ce as Ce oxide nanoparticles, which largely remained during the subsequent reductive dissolution of the Mn oxides. In addition, the XANES data indicate that goethite has the capability to oxidize Ce at near-neutral pH under our experimental conditions (goethite reacted with 0.001M Ce for 48 h in a glove box with O-2 < 1 ppm). This previously unrecognized Ce oxidation pathway also seems to contribute to a minor extent to the oxidative scavenging of Ce in the fracture network. Trivalent Ce in the fracture coatings, in particular below 2.5 m, is mainly sorbed as inner-sphere complexes on clay minerals. Taking into account the facts that Ce in the present groundwater is scarce and modeled to be largely complexed with humic substance, it is argued that the inner-sphere complexes were mainly formed from past (Paleozoic) hydrothermal fluids. (C) 2016 Elsevier Ltd. All rights reserved.

Keywords
Ce anomaly, Ce oxidation states, Oxidative scavenging, X-ray absorption near-edge structure
National Category
Geochemistry
Research subject
Natural Science
Identifiers
urn:nbn:se:lnu:diva-61146 (URN)10.1016/j.gca.2016.11.044 (DOI)000393125500023 ()
Available from: 2017-03-08 Created: 2017-03-08 Last updated: 2017-11-29Bibliographically approved
Yu, C., Drake, H., Dideriksen, K., Frandsen, C. & Åström, M. E. (2017). Iron speciation and valence in the upper 1 km of fractured crystalline bedrock on the Baltic shield. In: Goldschmidt2017 Abstracts: . Paper presented at Goldschmidt 2017 Paris.
Open this publication in new window or tab >>Iron speciation and valence in the upper 1 km of fractured crystalline bedrock on the Baltic shield
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2017 (English)In: Goldschmidt2017 Abstracts, 2017Conference paper, Poster (with or without abstract) (Refereed)
Abstract [en]

The widespread networks of open water-conducting fractures in crystalline bedrock are covered by a variety of Fe-bearing minerals. Quantitative information on Fe mineralogy and valence of these minerals is of great importance not only in constraining the biogeochemical cycle of Fe and other related elements in this largely unexplored space, but also in evaluating the mineralogical capacity to reduce oxygen which is one of the key issues in the risk assessment of nuclear waste repositories. 

Here, we studied Fe mineralogy and valence in fracture coatings, fresh rocks and altered rocks in the upper 1 km of fractured crystalline bedrock at two sites (Laxemar and Forsmark areas, Sweden) on the Baltic shield. Fe3+/∑Fe ratios in these materials were quantified based on the centroid position of the pre-edge feature on Fe XANES spectra, while the speciation of Fe was predicted by reconstructing the sample EXFAS spectra using a linear combination of a large dataset of reference spectra collected previously[1] and in this study. The results were compared with Mössbauer spectra. The fresh and altered rocks showed no systematic difference in Fe3+/∑Fe ratio, indicating that past hydrothermal activities (red-staining on fracture wall-rock) did not lead to a reduction in reducing capacity within the fracture networks. The fracture coatings from the Forsmark area are of clear hydrothermal character (as indicated by an abundance of hematite, hornblende and muscovite) and have not experienced the same degree of low-T oxidative weathering as the samples from the Laxemar area having frequent and abundant illite and ferrihydrite. However, Fe3+/∑Fe ratios of the fracture coatings from the two areas showed similar features, including no depth trend and a similar variability from 0.24-0.85 and 0.12-0.71 which are overall larger than the fresh and altered rocks. This suggests that regional geological events can have a significant impact on the speciation of Fe, but not Fe valence.

National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-76995 (URN)
Conference
Goldschmidt 2017 Paris
Available from: 2018-07-26 Created: 2018-07-26 Last updated: 2018-08-31Bibliographically approved
Yu, C., Peltola, P., Nystrand, M. I., Virtasalo, J. J., Österholm, P., Ojala, A. E. K., . . . Åström, M. E. (2016). Arsenic removal from contaminated brackish sea water by sorption onto Al hydroxides and Fe phases mobilized by land-use. Science of the Total Environment, 542, 923-934
Open this publication in new window or tab >>Arsenic removal from contaminated brackish sea water by sorption onto Al hydroxides and Fe phases mobilized by land-use
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2016 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 542, p. 923-934Article in journal (Refereed) Published
Abstract [en]

This study examines the spatial and temporal distribution patterns of arsenic (As) in solid and aqueous materials along the mixing zone of an estuary, located in the south-eastern part of the Bothnian Bay and fed by a creek running through an acid sulfate (AS) soil landscape. The concentrations of As in solution form (<1 kDa) increase steadily from the creek mouth to the outer estuary, suggesting that inflowing seawater, rather than AS soil, is the major As source in the estuary. In sediments at the outer estuary, As was accumulated and diagenetically cycled in the surficial layers, as throughout much of the Bothnian Bay. In contrast, in sediments in the inner estuary, As concentrations and accumulation rates showed systematical peaks at greater depths. These peaks were overall consistent with the temporal trend of past As discharges from the Ronnskar smelter and the accompanied As concentrations in past sea-water of the Bothnian Bay, pointing to a connection between the historical smelter activities and the sediment-bound As in the inner estuary. However, the concentrations and accumulation rates of As peaked at depths where the smelter activities had already declined, but a large increase in the deposition of Al hydroxides and Fe phases occurred in response to intensified land-use in the mid 1960's and early 1970's. This correspondence suggests that, apart from the inflowing As-contaminated seawater, capture by Al hydroxides, Fe hydroxides and Fe-organic complexes is another important factor for As deposition in the inner estuary. After accumulating in the sediment, the solid-phase As was partly remobilized, as reflected by increased pore-water As concentrations, a process favored by As(V) reduction and high concentrations of dissolved organic matter. (C) 2015 Elsevier B.V. All rights reserved.

Keywords
Arsenic, Estuarine sediments, The Bothnian Bay, Ronnskar smelter, Acid sulfate soils
National Category
Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
urn:nbn:se:lnu:diva-48801 (URN)10.1016/j.scitotenv.2015.11.013 (DOI)000365602100093 ()26558848 (PubMedID)2-s2.0-84946616230 (Scopus ID)
Available from: 2016-01-20 Created: 2016-01-15 Last updated: 2017-12-08Bibliographically approved
Nystrand, M. I., Österholm, P., Yu, C. & Åström, M. E. (2016). Distribution and speciation of metals, phosphorus, sulfate and organic material in brackish estuary water affected by acid sulfate soils. Applied Geochemistry, 66, 264-274
Open this publication in new window or tab >>Distribution and speciation of metals, phosphorus, sulfate and organic material in brackish estuary water affected by acid sulfate soils
2016 (English)In: Applied Geochemistry, ISSN 0883-2927, E-ISSN 1872-9134, Vol. 66, p. 264-274Article in journal (Refereed) Published
Abstract [en]

Dissolved (<1 kDa) and colloidal (1 kDa-0.45 mu m) size fractions of sulfate, organic carbon (OC), phosphate and 17 metals/metalloids were investigated in the acidic Vora River and its estuary in Western Finland. In addition, geochemical modelling was used to predict the formation of free ions and complexes in these waters. The sampling was carried out during high-water flow in autumn and in spring when the abundantly occurring acid sulfate (AS) soils in the catchment area are extensively flushed. Based on the high concentrations of sulfate, acidity and several metals, it is clear that the Vora River and its estuary is strongly affected by AS soils. The high dissolved form of metals limits also the existence of fish and other organisms in this estuary, and certainly also in other similar shallow brackish estuaries elsewhere in the Gulf of Bothnia. However, generally already <20% saline sea water reduces the concentration for OC and several elements (Al, Cu, Cr, Fe, Pb, PO4 and U) by half and c. 20-30% saline sea water is needed to halve concentrations of Cd, Co, Mn, Ni and Zn. Consequently, these elements as well as organic matters were rapidly precipitated in the estuary, even after mixing with fairly small amounts of the alkaline brackish sea water. Aluminium, Cu, Fe and U most likely precipitate together with organic matter closest to the river mouth. Manganese is relatively persistent in solution and, thus, precipitates further down the estuary as Mn oxides, which concomitantly capture Ba, Cd, Co, Cu, Ni and Zn. In the inner estuary, the high contents of Al is as important than Fe in removing PO4 and, thus, also reducing the risk of algae blooms in near coastal areas influenced by AS soils in the Gulf of Bothnia. Moreover, the dispersion of metals far out in the estuary is dependent on hydrological conditions, i.e. with high flows the plume of metal-rich water will spread further out in the estuary. Furthermore, the extensive drainage of the catchment and subsequent artificial enlargement of the river channel during recent decades has not only enabled oxidation of sulfidic sediments, but strongly increased flow peaks that reach further out in the estuary. (C) 2016 Elsevier Ltd. All rights reserved.

Keywords
Speciation, Ultrafiltration, Acid sulfate soil, Toxicity, Colloids, Estuary, Metals
National Category
Environmental Sciences
Research subject
Environmental Science, Environmental Chemistry
Identifiers
urn:nbn:se:lnu:diva-51063 (URN)10.1016/j.apgeochem.2016.01.003 (DOI)000370066400021 ()2-s2.0-84956652705 (Scopus ID)
External cooperation:
Available from: 2016-03-18 Created: 2016-03-18 Last updated: 2017-11-30Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-0635-3718

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