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1.
Artigo em Inglês | MEDLINE | ID: mdl-38766807

RESUMO

We set out to study the seasonal variations in porewater phosphorus and lanthanum concentrations in the dated sediment cores from a small eutrophic lake that has been treated with Phoslock, a lanthanum-modified bentonite (LMB) amendment. Three sites were sampled when the hypolimnion was either oxygenated or anoxic: (i) the lake's deepest point, (ii) a littoral site receiving inflows from the catchment, and (iii) a littoral site influenced by nearby septic tanks. Phosphate (PO43--P), lanthanum (La), iron (Fe), dissolved organic carbon (DOC) and sulfate (SO42-) were measured in porewater samples. An inverse diagenetic model was used to quantify fluxes of dissolved elements across the sediment-water interface as well as the net rate of their reactions along the porewater concentration gradients. Results show that porewater P and Fe underwent strong seasonal dynamics, while La did not. P fluxes, 20-fold higher at the deepest site than elsewhere in the basin, were influenced by anoxic conditions in the hypolimnion during summer and winter, suggesting that P mobility remained sensitive to redox fluctuations despite the addition of La. At the deepest site, fluxes of P across the sediment-water interface increased from 1 to 9 × 10-9 µmol cm-2 s-1 between spring and summer, while the rate of P production to the porewater also increased a hundredfold. These increases were concurrent with Fe mobilization. Finally, sediment dating shows that the fraction of P sequestered by La is buried under freshly deposited sediment at a rate of 2-3 mm per year. These results indicate that external P fluxes and erosion control remain crucial to maintain the longevity of the LMB treatment.

2.
J Environ Manage ; 324: 116410, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36352716

RESUMO

Floating solar photovoltaic (FPV) deployments are increasing globally as the switch to renewable energy intensifies, representing a considerable water surface transformation. FPV installations can potentially impact aquatic ecosystem function, either positively or negatively. However, these impacts are poorly resolved given the challenges of collecting empirical data for field or modelling experiments. In particular, there is limited evidence on the response of phytoplankton to changes in water body thermal dynamics and light climate with FPV. Given the importance of understanding phytoplankton biomass and species composition for managing ecosystem services, we use an uncertainty estimation approach to simulate the effect of FPV coverage and array siting location on a UK reservoir. FPV coverage was modified in 10% increments from a baseline with 0% coverage to 100% coverage for three different FPV array siting locations based on reservoir circulation patterns. Results showed that FPV coverage significantly impacted thermal properties, resulting in highly variable impacts on phytoplankton biomass and species composition. The impacts on phytoplankton were often dependent on array siting location as well as surface coverage. Changes to phytoplankton species composition were offset by the decrease in phytoplankton biomass associated with increasing FPV coverage. We identified that similar phytoplankton biomass reductions could be achieved with less FPV coverage by deploying the FPV array on the water body's faster-flowing area than the central or slower flowing areas. The difference in response dependent on siting location could be used to tailor phytoplankton management in water bodies. Simulation of water body-FPV interactions efficiently using an uncertainty approach is an essential tool to rapidly develop understanding and ultimately inform FPV developers and water body managers looking to minimise negative impacts and maximise co-benefits.


Assuntos
Ecossistema , Fitoplâncton , Biomassa , Luz Solar , Água
3.
Environ Sci Process Impacts ; 24(9): 1494-1507, 2022 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-35635543

RESUMO

Sustained eutrophication of the aquatic environment by the remobilization of legacy phosphorus (P) stored in soils and sediments is a prevailing issue worldwide. Fluxes of P from the sediments to the water column, referred to as internal P loading, often delays the recovery of water quality following a reduction in external P loads. Here, we report on the vertical distribution and geochemistry of P, lanthanum (La), iron (Fe) and carbon (C) in the culturally eutrophied Lake Bromont. This lake underwent remediation treatment using La modified bentonite (LMB) commercially available as Phoslock™. We investigated the effectiveness of LMB in decreasing soluble reactive phosphorus (SRP) availability in sediments and in reducing dissolved fluxes of P across the sediment-water interface. Sediment cores were retrieved before and after LMB treatment at three sites representing bottom sediment, sediment influenced by lakeside housing and finally littoral sediment influenced by the lake inflow. Sequential extractions were used to assess changes in P speciation. Depth profiles of dissolved porewater concentrations were obtained after LMB treatment at each site. Results indicate that SRP extracted from the sediments decreased at all sites, while total extracted P (PTOT) bound to redox-sensitive metal oxides increased. 31P NMR data on P extract reveals that 20-43% of total solid-phase P is in the form of organic P (Porg) susceptible to be released via microbial degradation. Geochemical modelling of porewater data provides evidence that LaPO4(s) mineral phases, such as rhabdophane and/or monazite, are likely forming. However, results also suggest that La3+ binding by dissolved organic carbon (DOC) hinders La-phosphate precipitation. We rely on thermodynamic modelling to suggest that high Fe2+ would bind to DOC instead of La3+, therefore promoting P sequestrations by LMB under anoxic conditions.


Assuntos
Lagos , Fósforo , Bentonita/química , Carbono , Argila , Sedimentos Geológicos/química , Ferro , Lagos/química , Lantânio/química , Fosfatos , Fósforo/química
4.
Environ Pollut ; 288: 117723, 2021 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-34256286

RESUMO

Lake sediments are widely used as environmental archives to reconstruct past changes in contaminants deposition, provided that they remain immobile after deposition. Arsenic (As) is a redox-sensitive element that may be redistributed in the sediments during early diagenesis, for instance along with iron and manganese, and thus depth profiles of As might not provide a reliable, unaltered record of past deposition. Here, we use inverse diagenetic modelling to calculate fluxes of As across the sediment-water interface and interpret As sedimentary records in eight lakes along a 80 km transect from the Giant and Con mines, Northwest Territories, Canada. The sediment cores were dated using 210Pb methods and analyzed for solid-phase and porewater As, Fe, Mn and organic C concentrations. We reconstructed the history of As deposition by correcting for the varying mobility patterns and calculated contemporary As deposition fluxes. Correction for diagenesis was substantial for three of the eight lakes, suggesting that lakes with lower sedimentation rates, which allows longer residence of As within the reactive zones defined by the model, enhance the influence of diagenesis. Results show that solid phase As peaks coincides with the period of high emissions from past gold ore roasting activities. Results also show that sediments sustained present-day As fluxes to the water column of study lakes within 50 km of the mines, while sediment in study lakes further than 50 km acted as As sinks instead.


Assuntos
Arsênio , Poluentes Químicos da Água , Arsênio/análise , Canadá , Monitoramento Ambiental , Sedimentos Geológicos , Ouro , Lagos , Poluentes Químicos da Água/análise
5.
Microbiome ; 9(1): 46, 2021 02 16.
Artigo em Inglês | MEDLINE | ID: mdl-33593438

RESUMO

BACKGROUND: The sulfur cycle encompasses a series of complex aerobic and anaerobic transformations of S-containing molecules and plays a fundamental role in cellular and ecosystem-level processes, influencing biological carbon transfers and other biogeochemical cycles. Despite their importance, the microbial communities and metabolic pathways involved in these transformations remain poorly understood, especially for inorganic sulfur compounds of intermediate oxidation states (thiosulfate, tetrathionate, sulfite, polysulfides). Isolated and highly stratified, the extreme geochemical and environmental features of meromictic ice-capped Lake A, in the Canadian High Arctic, provided an ideal model ecosystem to resolve the distribution and metabolism of aquatic sulfur cycling microorganisms along redox and salinity gradients. RESULTS: Applying complementary molecular approaches, we identified sharply contrasting microbial communities and metabolic potentials among the markedly distinct water layers of Lake A, with similarities to diverse fresh, brackish and saline water microbiomes. Sulfur cycling genes were abundant at all depths and covaried with bacterial abundance. Genes for oxidative processes occurred in samples from the oxic freshwater layers, reductive reactions in the anoxic and sulfidic bottom waters and genes for both transformations at the chemocline. Up to 154 different genomic bins with potential for sulfur transformation were recovered, revealing a panoply of taxonomically diverse microorganisms with complex metabolic pathways for biogeochemical sulfur reactions. Genes for the utilization of sulfur cycle intermediates were widespread throughout the water column, co-occurring with sulfate reduction or sulfide oxidation pathways. The genomic bin composition suggested that in addition to chemical oxidation, these intermediate sulfur compounds were likely produced by the predominant sulfur chemo- and photo-oxidisers at the chemocline and by diverse microbial degraders of organic sulfur molecules. CONCLUSIONS: The Lake A microbial ecosystem provided an ideal opportunity to identify new features of the biogeochemical sulfur cycle. Our detailed metagenomic analyses across the broad physico-chemical gradients of this permanently stratified lake extend the known diversity of microorganisms involved in sulfur transformations over a wide range of environmental conditions. The results indicate that sulfur cycle intermediates and organic sulfur molecules are major sources of electron donors and acceptors for aquatic and sedimentary microbial communities in association with the classical sulfur cycle. Video abstract.


Assuntos
Bactérias/genética , Bactérias/metabolismo , Ecossistema , Lagos/microbiologia , Metagenoma , Enxofre/metabolismo , Organismos Aquáticos/genética , Organismos Aquáticos/metabolismo , Canadá , Oxirredução
6.
Nat Ecol Evol ; 4(8): 1060-1068, 2020 08.
Artigo em Inglês | MEDLINE | ID: mdl-32541802

RESUMO

Climate and land-use change drive a suite of stressors that shape ecosystems and interact to yield complex ecological responses (that is, additive, antagonistic and synergistic effects). We know little about the spatial scales relevant for the outcomes of such interactions and little about effect sizes. These knowledge gaps need to be filled to underpin future land management decisions or climate mitigation interventions for protecting and restoring freshwater ecosystems. This study combines data across scales from 33 mesocosm experiments with those from 14 river basins and 22 cross-basin studies in Europe, producing 174 combinations of paired-stressor effects on a biological response variable. Generalized linear models showed that only one of the two stressors had a significant effect in 39% of the analysed cases, 28% of the paired-stressor combinations resulted in additive effects and 33% resulted in interactive (antagonistic, synergistic, opposing or reversal) effects. For lakes, the frequencies of additive and interactive effects were similar for all spatial scales addressed, while for rivers these frequencies increased with scale. Nutrient enrichment was the overriding stressor for lakes, with effects generally exceeding those of secondary stressors. For rivers, the effects of nutrient enrichment were dependent on the specific stressor combination and biological response variable. These results vindicate the traditional focus of lake restoration and management on nutrient stress, while highlighting that river management requires more bespoke management solutions.


Assuntos
Ecossistema , Água Doce , Biota , Europa (Continente) , Rios
7.
Proc Natl Acad Sci U S A ; 117(21): 11566-11572, 2020 05 26.
Artigo em Inglês | MEDLINE | ID: mdl-32385161

RESUMO

Large-scale and rapid improvement in wastewater treatment is common practice in developing countries, yet this influence on nutrient regimes in receiving waterbodies is rarely examined at broad spatial and temporal scales. Here, we present a study linking decadal nutrient monitoring data in lakes with the corresponding estimates of five major anthropogenic nutrient discharges in their surrounding watersheds over time. Within a continuous monitoring dataset covering the period 2008 to 2017, we find that due to different rates of change in TN and TP concentrations, 24 of 46 lakes, mostly located in China's populated regions, showed increasing TN/TP mass ratios; only 3 lakes showed a decrease. Quantitative relationships between in-lake nutrient concentrations (and their ratios) and anthropogenic nutrient discharges in the surrounding watersheds indicate that increase of lake TN/TP ratios is associated with the rapid improvement in municipal wastewater treatment. Due to the higher removal efficiency of TP compared with TN, TN/TP mass ratios in total municipal wastewater discharge have continued to increase from a median of 10.7 (95% confidence interval, 7.6 to 15.1) in 2008 to 17.7 (95% confidence interval, 13.2 to 27.2) in 2017. Improving municipal wastewater collection and treatment worldwide is an important target within the 17 sustainable development goals set by the United Nations. Given potential ecological impacts on biodiversity and ecosystem function of altered nutrient ratios in wastewater discharge, our results suggest that long-term strategies for domestic wastewater management should not merely focus on total reductions of nutrient discharges but also consider their stoichiometric balance.


Assuntos
Lagos/química , Nitrogênio/análise , Fósforo/análise , Águas Residuárias/química , Purificação da Água , China , Ecossistema , Monitoramento Ambiental , Purificação da Água/métodos , Purificação da Água/normas , Qualidade da Água/normas
8.
Sci Total Environ ; 713: 136549, 2020 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-31954242

RESUMO

Lake Auburn, Maine, USA, is a historically unproductive lake that has experienced multiple algal blooms since 2011. The lake is the water supply source for a population of ~60,000. We modeled past temperature, and concentrations of dissolved oxygen (DO) and phosphorus (P) in Lake Auburn by considering the catchment and internal contributions of P as well as atmospheric factors, and predicted the change in lake water quality in response to future climate and land-use changes. A stream hydrology and P-loading model (SimplyP) was used to generate input from two major tributaries into a lake model (MyLake-Sediment) to simulate physical mixing, chemical dynamics, and sediment geochemistry in Lake Auburn from 2013 to 2017. Simulations of future lake water quality were conducted using meteorological boundary conditions derived from recent historical data and climate model projections for high greenhouse-gas emission cases. The effects of future land development on lake water quality for the 2046 to 2055 time period under different land-use and climate change scenarios were also simulated. Our results indicate that lake P enrichment is more responsive to extreme storm events than increasing air temperatures, mean precipitation, or windstorms; loss of fish habitat is driven by windstorms, and to a lesser extent an increasing water temperature; and catchment development further leads to water quality decline. All simulations also show that the lake is susceptible to both internal and external P loadings. Simulation of temperature, DO, and P proved to be an effective means for predicting the loss of water quality under changing land-use and climate scenarios.

9.
Bull Environ Contam Toxicol ; 103(1): 69-74, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30937495

RESUMO

Waste tanks at the nuclear facility located at Sellafield, UK, represent a nuclear source which could release radionuclides to the atmosphere. A model chain which combines atmospheric transport, deposition as well as riverine transport to sea has been developed to predict the riverine activity concentrations of 137Cs. The source term was estimated to be 9 × 104 TBq of 137Cs, or 1% of the assumed total 137Cs inventory of the HAL (Highly Active Liquid) storage tanks. Air dispersion modelling predicted 137Cs deposition reaching 127 kBq m-2 at the Vikedal catchment in Western Norway. Thus, the riverine transport model predicted that the activity concentration of 137Cs in water at the river outlet could reach 9000 Bq m-3 in the aqueous phase and 1000 Bq kg-1 in solid phase at peak level. The lake and river reaches showed different transport patterns due to the buffering effects caused by dilution and slowing down of water velocity.


Assuntos
Radioisótopos de Césio/análise , Modelos Químicos , Monitoramento de Radiação , Resíduos Radioativos , Poluentes Radioativos do Ar/análise , Atmosfera , Noruega , Rios , Poluentes Radioativos da Água/análise
10.
Sci Total Environ ; 668: 470-484, 2019 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-30852223

RESUMO

There are infinite possible future scenarios reflecting the impacts of anthropogenic multiple stress on our planet. These impacts include changes in climate and land cover, to which aquatic ecosystems are especially vulnerable. To assess plausible developments of the future state of European surface waters, we considered two climate scenarios and three storylines describing land use, management and anthropogenic development ('Consensus', 'Techno' and 'Fragmented', which in terms of environmental protection represent best-, intermediate- and worst-case, respectively). Three lake and four river basins were selected, representing a spectrum of European conditions through a range of different human impacts and climatic, geographical and biological characteristics. Using process-based and empirical models, freshwater total nitrogen, total phosphorus and chlorophyll-a concentrations were projected for 2030 and 2060. Under current conditions, the water bodies mostly fail good ecological status. In future predictions for the Techno and Fragmented World, concentrations further increased, while concentrations generally declined for the Consensus World. Furthermore, impacts were more severe for rivers than for lakes. Main pressures identified were nutrient inputs from agriculture, land use change, inadequately managed water abstractions and climate change effects. While the basins in the Continental and Atlantic regions were primarily affected by land use changes, in the Mediterranean/Anatolian the main driver was climate change. The Boreal basins showed combined impacts of land use and climate change and clearly reflected the climate-induced future trend of agricultural activities shifting northward. The storylines showed positive effects on ecological status by classical mitigation measures in the Consensus World (e.g. riparian shading), technical improvements in the Techno World (e.g. increasing wastewater treatment efficiency) and agricultural extensification in the Fragmented World. Results emphasize the need for implementing targeted measures to reduce anthropogenic impacts and the importance of having differing levels of ambition for improving the future status of water bodies depending on the societal future to be expected.

11.
Sci Total Environ ; 663: 718-730, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-30731417

RESUMO

The impact of seasonal fluctuations linked to monsoon and irrigation generates redox oscillations in the subsurface, influencing the release of arsenic (As) in aquifers. Here, the biogeochemical control on As mobility was investigated in batch experiments using redox cycling bioreactors and As- and SO42--amended sediment. Redox potential (Eh) oscillations between anoxic (-300-0 mV) and oxic condition (0-500 mV) were implemented by automatically modulating an admixture of N2/CO2 or compressed air. A carbon source (cellobiose, a monomer of cellulose) was added at the beginning of each reducing cycle to stimulate the metabolism of the native microbial community. Results show that successive redox cycles can decrease arsenic mobility by up to 92% during reducing conditions. Anoxic conditions drive mainly the conversion of soluble As(V) to As(III) in contrast to oxic conditions. Phylogenetic analyses of 16S rRNA amplified from the sediments revealed the presence of sulfate and iron - reducing bacteria, confirming that sulfate and iron reduction are key factors for As immobilization from the aqueous phase. As and S K-edge X-ray absorption spectroscopy suggested the association of Fe-(oxyhydr)oxides and the importance of pyrite (FeS2(s)), rather than poorly ordered mackinawite (FeS(s)), for As sequestration under oxidizing and reducing conditions, respectively. Finally, these findings suggest a role for elemental sulfur in mediating aqueous thioarsenates formation in As-contaminated groundwater of the Mekong delta.


Assuntos
Arsênio/análise , Bactérias/metabolismo , Monitoramento Ambiental , Água Subterrânea/química , Sulfatos/metabolismo , Poluentes Químicos da Água/análise , Reatores Biológicos , Oxirredução , Vietnã , Espectroscopia por Absorção de Raios X
12.
Sci Total Environ ; 627: 733-743, 2018 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-29426198

RESUMO

Interactions between climate change and land use change might have substantial effects on aquatic ecosystems, but are still poorly understood. Using the Welsh River Wye as a case study, we linked models of water quality (Integrated Catchment - INCA) and climate (GFDL - Geophysical Fluid Dynamics Laboratory and IPSL - Institut Pierre Simon Laplace) under greenhouse gas scenarios (RCP4.5 and RCP8.5) to drive a bespoke ecosystem model that simulated the responses of aquatic organisms. The potential effects of economic and social development were also investigated using scenarios from the EU MARS project (Managing Aquatic Ecosystems and Water Resources under Multiple Stress). Longitudinal position along the river mediated response to increasing anthropogenic pressures. Upland locations appeared particularly sensitive to nutrient enrichment or potential re-acidification compared to lowland environments which are already eutrophic. These results can guide attempts to mitigate future impacts and reiterate the need for sensitive land management in upland, temperate environments which are likely to become increasingly important to water supply and biodiversity conservation as the effects of climate change intensify.


Assuntos
Mudança Climática , Ecossistema , Monitoramento Ambiental/métodos , Modelos Teóricos , Rios/química , Ecologia , Guanina/análogos & derivados , País de Gales
13.
Environ Sci Process Impacts ; 20(2): 406-414, 2018 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-29359225

RESUMO

Thousands of boreal lakes were limed for decades in Scandinavia to counteract the effect of anthropogenic acidification. We measured the concentrations of alkali earth metals (Ca, Mg, Ba), metals (Mn, Fe, Al, Co, Cd, Pb, Zn), metalloids (As, Mo) and phosphorus (P) in 165 surface sediment samples from 17 limed lakes, as well as the sediment column and porewater of two lakes chosen from this set. We report that formation of ferromanganese nodules is widespread in limed lakes, and that those nodules are enriched in trace elements, reaching for example 11 500, 908 and 40 µg g-1 for Ba, Mo and As, respectively. Nodules are more abundant between the littoral and the profundal zones. Intense redox cycling of Fe and Mn at the sediment-water interface has redistributed trace elements in the sediment column. Ba, Co, Mo, Pb and Zn partitioned with Mn (oxy)hydroxides and As and P with Fe (oxy)hydroxides. Fe, Mo, Co and As remobilized to the porewater also diffused downward and were likely sequestrated with sulfides. We conclude that the diagenetic redistribution and partitioning of trace elements onto Fe-Mn nodules, rather than direct inputs from liming, is the cause of the elevated trace element burden in surface sediments.


Assuntos
Monitoramento Ambiental/métodos , Sedimentos Geológicos/química , Ferro/análise , Lagos/química , Manganês/análise , Oligoelementos/análise , Poluentes Químicos da Água/análise , Compostos de Cálcio/química , Concentração de Íons de Hidrogênio , Metais Pesados/análise , Modelos Teóricos , Noruega , Óxidos/química , Termodinâmica
14.
Sci Total Environ ; 621: 713-724, 2018 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-29197290

RESUMO

Excess nutrient inputs and climate change are two of multiple stressors affecting many lakes worldwide. Lake Vansjø in southern Norway is one such eutrophic lake impacted by blooms of toxic blue-green algae (cyanobacteria), and classified as moderate ecological status under the EU Water Framework Directive. Future climate change may exacerbate the situation. Here we use a set of chained models (global climate model, hydrological model, catchment phosphorus (P) model, lake model, Bayesian Network) to assess the possible future ecological status of the lake, given the set of climate scenarios and storylines common to the EU project MARS (Managing Aquatic Ecosystems and Water Resources under Multiple Stress). The model simulations indicate that climate change alone will increase precipitation and runoff, and give higher P fluxes to the lake, but cause little increase in phytoplankton biomass or changes in ecological status. For the storylines of future management and land-use, however, the model results indicate that both the phytoplankton biomass and the lake ecological status can be positively or negatively affected. Our results also show the value in predicting a biological indicator of lake ecological status, in this case, cyanobacteria biomass with a BN model. For all scenarios, cyanobacteria contribute to worsening the status assessed by phytoplankton, compared to using chlorophyll-a alone.


Assuntos
Mudança Climática , Eutrofização , Lagos/análise , Modelos Teóricos , Qualidade da Água , Teorema de Bayes , Cianobactérias , Noruega , Fitoplâncton
15.
Sci Total Environ ; 574: 128-138, 2017 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-27627688

RESUMO

Many surface waters in Europe suffer from the adverse effects of multiple stresses. The Otra River, southernmost Norway, is impacted by acid deposition, hydropower development and increasingly by climate change. The river holds a unique population of land-locked salmon and anadromous salmon in the lower reaches. Both populations have been severely affected by acidification. The decrease in acid deposition since the 1980s has led to partial recovery of both populations. Climate change with higher temperatures and altered precipitation can potentially further impact fish populations. We used a linked set of process-oriented models to simulate future climate, discharge, and water chemistry at five sub-catchments in the Otra river basin. Projections to year 2100 indicate that future climate change will give a small but measureable improvement in water quality, but that additional reductions in acid deposition are needed to promote full restoration of the fish communities. These results can help guide management decisions to sustain key salmon habitats and carry out effective long-term mitigation strategies such as liming. The Otra River is typical of many rivers in Europe in that it fails to achieve the good ecological status target of the EU Water Framework Directive. The programme of measures needed in the river basin management plan necessarily must consider the multiple stressors of acid deposition, hydropower, and climate change. This is difficult, however, as the synergistic and antagonistic effects are complex and challenging to address with modelling tools currently available.


Assuntos
Mudança Climática , Monitoramento Ambiental , Energia Renovável , Rios/química , Salmão , Ácidos/análise , Animais , Concentração de Íons de Hidrogênio , Noruega
16.
Environ Sci Technol ; 50(14): 7610-7, 2016 07 19.
Artigo em Inglês | MEDLINE | ID: mdl-27309856

RESUMO

We assessed the potential of zerovalent-iron- (Fe(0)) based permeable reactive barrier (PRB) systems for arsenic (As) remediation in the presence or absence of microbial sulfate reduction. We conducted long-term (200 day) flow-through column experiments to investigate the mechanisms of As transformation and mobility in aquifer sediment (in particular, the PRB downstream linkage). Changes in As speciation in the aqueous phase were monitored continuously. Speciation in the solid phase was determined at the end of the experiment using X-ray absorption near-edge structure (XANES) spectroscopy analysis. We identified thio-As species in solution and AsS in solid phase, which suggests that the As(V) was reduced to As(III) and precipitated as AsS under sulfate-reducing conditions and remained as As(V) under abiotic conditions, even with low redox potential and high Fe(II) content (4.5 mM). Our results suggest that the microbial sulfate reduction plays a key role in the mobilization of As from Fe-rich aquifer sediment under anoxic conditions. Furthermore, they illustrate that the upstream-downstream linkage of PRB affects the speciation and mobility of As in downstream aquifer sediment, where up to 47% of total As initially present in the sediment was leached out in the form of mobile thio-As species.


Assuntos
Arsênio/química , Ferro/química , Oxirredução , Sulfatos/química , Raios X
17.
Environ Sci Technol ; 49(5): 3015-23, 2015 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-25633742

RESUMO

Near-surface biogeochemical systems can oscillate between oxic and anoxic conditions. Under such periodic changes many redox-sensitive inorganic contaminants undergo speciation, mobility and toxicity changes. We investigated the changes to chromium (Cr), arsenic (As), selenium (Se), antimony (Sb) and uranium (U) mobility during a series of laboratory experiments where argillaceous substrates were subjected to successive cycles of oxidizing and reducing conditions. The EH oscillated between -320 and +470 mV, induced via both abiotic and microbial forcings. Chemically induced cycles of oxidation and reduction were achieved via a combination of gas (N2:CO2 vs compressed air) and carbon (ethanol) addition, to stimulate the metabolism of a natively present microbial community. The contaminants were added either alone or as contaminant mixtures. Results show clear on-off switch mobility behavior for both major elements such as carbon (C), iron (Fe) and manganese (Mn) and for contaminants. Mn, Fe, and As were mobilized under anoxic conditions, whereas Sb, Se, and U were mobilized under oxic conditions. While As, Sb, and U were reversibly sorbed, Se and Cr were irreversibly sequestered via reductive precipitation. When present in aqueous solutions at high concentrations, Cr(VI) prevented the reduction of Mn and Fe, and inhibited the mobilization of elements with lower EH(o). To improve remediation strategies for multiple contaminants in redox-dynamic environments, we propose a mixed kinetic-equilibrium biogeochemical model that can be forced by oscillating boundary conditions and that uses literature rates and constants to capture the key processes responsible for the mobilization of contaminants in soils.


Assuntos
Metais Pesados/análise , Poluentes do Solo/análise , Solo/química , Carbono/química , Ecologia , Oxirredução
18.
Environ Sci Technol ; 48(17): 10174-81, 2014 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-25072630

RESUMO

Field measurements combined with numerical simulations provide insight into the water exchange, groundwater flow, and geochemical processes controlling the mobility of arsenic (As) in freshwater beach aquifers. Elevated dissolved As (up to 56 µg/L) was observed 1-2 m below the shoreline at two sandy beaches on Lake Erie, Ontario, Canada. Water and solid-phase analyses suggest that Fe (hydr)oxides present below the shoreline accumulate As, creating a risk of high As in the beach aquifer. Groundwater flow simulations combined with vertical hydraulic gradient measurements indicate that wave-induced flow recirculations across the groundwater-lake interface are significant. These recirculations, which vary with wave intensity and lake water level fluctuations, set up redox and pH gradients, where Fe precipitates and subsequently sequesters As. The elevated As concentrations observed at both beaches, combined with the distribution of other dissolved species, suggest that the As enrichment may be naturally occurring. Regardless of the As source, the interacting hydrologic and geochemical processes revealed may have important implications for the flux of As and also other oxyanions, such as phosphate, across the groundwater-lake interface in nearshore areas of the Great Lakes.


Assuntos
Arsênio/análise , Praias , Água Subterrânea/química , Lagos/química , Canadá , Sedimentos Geológicos/química , Concentração de Íons de Hidrogênio , Reologia , Soluções , Poluentes Químicos da Água/análise
19.
Environ Sci Process Impacts ; 16(7): 1588-99, 2014 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-24622900

RESUMO

A model network comprising climate models, a hydrological model, a catchment-scale model for phosphorus biogeochemistry, and a lake thermodynamics and plankton dynamics model was used to simulate phosphorus loadings, total phosphorus and chlorophyll concentrations in Lake Vansjø, Southern Norway. The model network was automatically calibrated against time series of hydrological, chemical and biological observations in the inflowing river and in the lake itself using a Markov Chain Monte-Carlo (MCMC) algorithm. Climate projections from three global climate models (GCM: HadRM3, ECHAM5r3 and BCM) were used. The GCM model HadRM3 predicted the highest increase in temperature and precipitation and yielded the highest increase in total phosphorus and chlorophyll concentrations in the lake basin over the scenario period of 2031-2060. Despite the significant impact of climate change on these aspects of water quality, it is minimal when compared to the much larger effect of changes in land-use. The results suggest that implementing realistic abatement measures will remain a viable approach to improving water quality in the context of climate change.


Assuntos
Agricultura , Mudança Climática , Eutrofização , Lagos/química , Modelos Químicos , Fósforo/análise , Poluentes Químicos da Água/análise , Poluição Química da Água/estatística & dados numéricos , Monitoramento Ambiental , Hidrologia , Noruega , Rios , Movimentos da Água
20.
Appl Environ Microbiol ; 79(14): 4325-35, 2013 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-23666325

RESUMO

Microcosms containing sediment from an aquifer in Cambodia with naturally elevated levels of arsenic in the associated groundwater were used to evaluate the effectiveness of microbially mediated production of iron minerals for in situ As remediation. The microcosms were first incubated without amendments for 28 days, and the release of As and other geogenic chemicals from the sediments into the aqueous phase was monitored. Nitrate or a mixture of sulfate and lactate was then added to stimulate biological Fe(II) oxidation or sulfate reduction, respectively. Without treatment, soluble As concentrations reached 3.9 ± 0.9 µM at the end of the 143-day experiment. However, in the nitrate- and sulfate-plus-lactate-amended microcosms, soluble As levels decreased to 0.01 and 0.41 ± 0.13 µM, respectively, by the end of the experiment. Analyses using a range of biogeochemical and mineralogical tools indicated that sorption onto freshly formed hydrous ferric oxide (HFO) and iron sulfide mineral phases are the likely mechanisms for As removal in the respective treatments. Incorporation of the experimental results into a one-dimensional transport-reaction model suggests that, under conditions representative of the Cambodian aquifer, the in situ precipitation of HFO would be effective in bringing groundwater into compliance with the World Health Organization (WHO) provisional guideline value for As (10 ppb or 0.13 µM), although soluble Mn release accompanying microbial Fe(II) oxidation presents a potential health concern. In contrast, production of biogenic iron sulfide minerals would not remediate the groundwater As concentration below the recommended WHO limit.


Assuntos
Arsênio/metabolismo , Bactérias/metabolismo , Compostos Férricos/metabolismo , Compostos de Ferro/metabolismo , Poluentes Químicos da Água/metabolismo , Bactérias/classificação , Bactérias/genética , Biodegradação Ambiental , Camboja , Sedimentos Geológicos/química , Sedimentos Geológicos/microbiologia , Água Subterrânea/química , Água Subterrânea/microbiologia , Modelos Químicos , Dados de Sequência Molecular , Filogenia , RNA Bacteriano/genética , RNA Bacteriano/metabolismo , RNA Ribossômico 16S/genética , RNA Ribossômico 16S/metabolismo
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