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1.
Environ Microbiol ; 26(1): e16558, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38115223

RESUMEN

Subterranean estuaries (STEs) are important coastal biogeochemical reactors facilitating unique niches for microbial communities. A common approach in determining STE greenhouse gas and nutrient fluxes is to use terrestrial endmembers, not accounting for microbially mediated transformations throughout the STE. As such, the microbial ecology and spatial distribution of specialists that cycle compounds in STEs remain largely underexplored. In this study, we applied 16S rRNA amplicon sequencing with paired biogeochemical characterisations to spatially evaluate microbial communities transforming greenhouse gases and nutrients in an STE. We show that methanogens are most prevalent at the terrestrial end (up to 2.81% relative abundance) concomitant to the highest porewater methane, carbon dioxide and dissolved organic carbon concentrations (0.41 ± 0.02 µM, 273.31 ± 6.05 µM and 0.51 ± 0.02 mM, respectively). Lower ammonium concentrations corresponded with abundant nitrifying and ammonia-oxidising prokaryotes in the mixing zone (up to 11.65% relative abundance). Methane, ammonium and dissolved organic carbon concentrations all decreased by >50% from the terrestrial to the oceanic end of the 15 m transect. This study highlights the STE's hidden microbiome zonation, as well as the importance of accounting for microbial transformations mitigating nutrient and greenhouse gas fluxes to the coastal ecosystems.


Asunto(s)
Compuestos de Amonio , Gases de Efecto Invernadero , Microbiota , Estuarios , Metano , Materia Orgánica Disuelta , Nitrógeno , ARN Ribosómico 16S/genética , Microbiota/genética
2.
New Phytol ; 242(1): 49-60, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-37984803

RESUMEN

Tree stem methane emissions are important components of lowland forest methane budgets. The potential for species-specific behaviour among co-occurring lowland trees with contrasting bark characteristics has not been investigated. We compare bark-mediated methane transport in two common lowland species of contrasting bark characteristics (Melaleuca quinquenervia featuring spongy/layered bark with longitudinally continuous airspaces and Casuarina glauca featuring hard/dense common bark) through several manipulative experiments. First, the progressive cutting through M. quinquenervia bark layers caused exponential increases in methane fluxes (c. 3 orders of magnitude); however, sapwood-only fluxes were lower, suggesting that upward/axial methane transport occurs between bark layers. Second, concentrated methane pulse-injections into exposed M. quinquenervia bark, revealed rapid axial methane transport rates (1.42 mm s-1 ), which were further supported through laboratory-simulated experiments (1.41 mm s-1 ). Laboratory-simulated radial CH4 diffusion rates (through bark) were c. 20-times slower. Finally, girdling M. quinquenervia stems caused a near-instantaneous decrease in methane flux immediately above the cut. By contrast, girdling C. glauca displayed persistent, though diminished, methane fluxes. Overall, the experiments revealed evidence for rapid 'between-bark' methane transport independent from the transpiration stream in M. quinquenervia, which facilitates diffusive axial transport from the rhizosphere and/or sapwood sources. This contrasts with the slower, radial 'through-bark' diffusive-dominated gas transportation in C. glauca.


Asunto(s)
Melaleuca , Árboles , Metano , Corteza de la Planta , Bosques , Dióxido de Carbono , Suelo
3.
MMWR Morb Mortal Wkly Rep ; 72(38): 1032-1040, 2023 Sep 22.
Artículo en Inglés | MEDLINE | ID: mdl-37733637

RESUMEN

Mental and behavioral health conditions among school-aged children, including substance use disorders and overall emotional well-being, are a public health concern in the United States. Timely data on seasonal patterns in child and adolescent conditions can guide optimal timing of prevention and intervention strategies. CDC examined emergency department (ED) visit data from the National Syndromic Surveillance Program for 25 distinct conditions during January 2018-June 2023 among U.S. children and adolescents aged 5-17 years, stratified by age group. Each year, during 2018-2023, among persons aged 10-14 and 15-17 years, the number and proportion of weekly ED visits for eight conditions increased in the fall school semester and remained elevated throughout the spring semester; ED visits were up to twice as high during school semesters compared with the summer period. Among children aged 5-9 years, the number and proportion of visits increased for five mental and behavioral health conditions. Seasonal increases in ED visits for some conditions among school-aged children warrant enhanced awareness about mental distress symptoms and the challenges and stressors in the school environment. Systemic changes that prioritize protective factors (e.g., physical activity; nutrition; sleep; social, community, or faith-based support; and inclusive school and community environments) and incorporate preparedness for increases in conditions during back-to-school planning might improve child and adolescent mental health.


Asunto(s)
Servicio de Urgencia en Hospital , Trastornos Mentales , Salud Mental , Adolescente , Niño , Humanos , Trastornos Mentales/epidemiología , Trastornos Mentales/terapia , Estaciones del Año , Estados Unidos/epidemiología
4.
Environ Sci Technol ; 57(12): 4813-4820, 2023 03 28.
Artículo en Inglés | MEDLINE | ID: mdl-36929871

RESUMEN

Jarosite, a common mineral in acidic sulfur-rich environments, can strongly sorb both As(V) and Sb(V). However, little is known regarding the mechanisms that control simultaneous co-sorption of As(V) and Sb(V) to jarosite. We investigated the mechanisms controlling As(V) and Sb(V) sorption to jarosite at pH 3 (in dual and single metalloid treatments). Jarosite was found to sorb Sb(V) to a greater extent than As(V) in both single and dual metalloid treatments. Relative to single metalloid treatments, the dual presence of both As(V) and Sb(V) decreased the sorption of both metalloids by almost 50%. Antimony K-edge EXAFS spectroscopy revealed that surface precipitation of an Sb(V) oxide species was the predominant sorption mechanism for Sb(V). In contrast, As K-edge EXAFS spectroscopy showed that As(V) sorption occurred via bidentate corner-sharing complexes on the jarosite surface when Sb(V) was absent or present at low loadings or by formation of similar complexes on the Sb(V) oxide surface precipitate when Sb(V) was present at high loadings. These results point to a novel mechanism by which Sb(V) impacts the co-sorption of As(V). Overall, these findings highlight a strong contrast in the sorption mechanisms of Sb(V) versus As(V) to jarosite under acidic environmental conditions.


Asunto(s)
Arsénico , Arsénico/química , Antimonio/química , Rayos X , Adsorción , Óxidos , Espectroscopía de Absorción de Rayos X
5.
Environ Sci Technol ; 56(24): 17776-17784, 2022 12 20.
Artículo en Inglés | MEDLINE | ID: mdl-36445713

RESUMEN

This study examines incorporation of Sb(V) into schwertmannite─an Fe(III) oxyhydroxysulfate mineral that can be an important Sb host phase in acidic environments. Schwertmannite was synthesized from solutions containing a range of Sb(V)/Fe(III) ratios, and the resulting solids were investigated using geochemical analysis, powder X-ray diffraction (XRD), dissolution kinetic experiments, and extended X-ray absorption fine structure (EXAFS) spectroscopy. Shell-fitting and wavelet transform analyses of Sb K-edge EXAFS data, together with congruent Sb and Fe release during schwertmannite dissolution, indicate that schwertmannite incorporates Sb(V) via heterovalent substitution for Fe(III). Elemental analysis combined with XRD and Fe K-edge EXAFS spectroscopy shows that schwertmannite can incorporate Sb(V) via this mechanism at up to about 8 mol % substitution when formed from solutions having Sb/Fe ratios ≤0.04 (higher ratios inhibit schwertmannite formation). Incorporation of Sb(V) into schwertmannite involves formation of edge and double-corner sharing linkages between SbVO6 and FeIII(O,OH)6 octahedra which strongly stabilize schwertmannite against dissolution. This implies that Sb(V)-coprecipitated schwertmannite may represent a potential long-term sink for Sb in acidic environments.


Asunto(s)
Compuestos Férricos , Compuestos de Hierro , Compuestos Férricos/química , Antimonio/química , Compuestos de Hierro/química , Compuestos de Hierro/metabolismo , Minerales/química , Adsorción , Oxidación-Reducción
6.
New Phytol ; 230(6): 2200-2212, 2021 06.
Artículo en Inglés | MEDLINE | ID: mdl-33715152

RESUMEN

Knowledge regarding mechanisms moderating methane (CH4 ) sink/source behaviour along the soil-tree stem-atmosphere continuum remains incomplete. Here, we applied stable isotope analysis (δ13 C-CH4 ) to gain insights into axial CH4 transport and oxidation in two globally distributed subtropical lowland species (Melaleuca quinquenervia and Casuarina glauca). We found consistent trends in CH4 flux (decreasing with height) and δ13 C-CH4 enrichment (increasing with height) in relation to stem height from ground. The average lower tree stem δ13 C-CH4 (0-40 cm) of Melaleuca and Casuarina (-53.96‰ and -65.89‰) were similar to adjacent flooded soil CH4 ebullition (-52.87‰ and -62.98‰), suggesting that stem CH4 is derived mainly by soil sources. Upper stems (81-200 cm) displayed distinct δ13 C-CH4 enrichment (Melaleuca -44.6‰ and Casuarina -46.5‰, respectively). Coupled 3D-photogrammetry with novel 3D-stem measurements revealed distinct hotspots of CH4 flux and isotopic fractionation on Melaleuca, which were likely due to bark anomalies in which preferential pathways of gas efflux were enhanced. Diel experiments revealed greater δ13 C-CH4 enrichment and higher oxidation rates in the afternoon, compared with the morning. Overall, we estimated that c. 33% of the methane was oxidised between lower and upper stems during axial transport, therefore potentially representing a globally significant, yet previously unaccounted for, methane sink.


Asunto(s)
Metano , Árboles , Atmósfera , Bosques , Suelo
7.
Environ Sci Technol ; 55(14): 9854-9863, 2021 07 20.
Artículo en Inglés | MEDLINE | ID: mdl-34228928

RESUMEN

Manganese (Mn) oxides, such as birnessite (δ-MnO2), are ubiquitous mineral phases in soils and sediments that can interact strongly with antimony (Sb). The reaction between birnessite and aqueous Mn(II) can induce the formation of secondary Mn oxides. Here, we studied to what extent different loadings of antimonate (herein termed Sb(V)) sorbed to birnessite determine the products formed during Mn(II)-induced transformation (at pH 7.5) and corresponding changes in Sb behavior. In the presence of 10 mM Mn(II)aq, low Sb(V)aq (10 µmol L-1) triggered the transformation of birnessite to a feitknechtite (ß-Mn(III)OOH) intermediary phase within 1 day, which further transformed into manganite (γ-Mn(III)OOH) over 30 days. Medium and high concentrations of Sb(V)aq (200 and 600 µmol L-1, respectively) led to the formation of manganite, hausmannite (Mn(II)Mn(III)2O4), and groutite (αMn(III)OOH). The reaction of Mn(II) with birnessite enhanced Sb(V)aq removal compared to Mn(II)-free treatments. Antimony K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy revealed that heterovalent substitution of Sb(V) for Mn(III) occurred within the secondary Mn oxides, which formed via the Mn(II)-induced transformation of Sb(V)-sorbed birnessite. Overall, Sb(V) strongly influenced the products of the Mn(II)-induced transformation of birnessite, which in turn attenuated Sb mobility via incorporation of Sb(V) within the secondary Mn oxide phases.


Asunto(s)
Compuestos de Manganeso , Óxidos , Adsorción , Concentración de Iones de Hidrógeno , Manganeso , Oxidación-Reducción
8.
Br J Hist Sci ; 54(2): 155-175, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-33739248

RESUMEN

This article presents a case study of life and work at the Royal Observatory at Greenwich (1835-1933) which reveals tensions between the lived reality of the observatory as a social space, and the attempts to create order, maintain discipline and project an image of authority in order to ensure the observatory's long-term stability. Domestic, social and scientific activities all intermingled within the observatory walls in ways which were occasionally disorderly. But life at Greenwich was carefully managed to stave off such disorder and to maintain an appearance of respectability which was essential to the observatory's reputation and output. The article focuses on three areas of management: (1) the observatory's outer boundaries, demonstrating how Greenwich navigated both human and environmental intrusions from the wider world; (2) the house, examining how Greenwich's domestic spaces provided stability, while also complicating observatory life via the management of domestic servants; and (3) the scientific spaces, with an emphasis on the work and play of the observatory's boy computers. Together, these three parts demonstrate that the stability of the observatory was insecure, despite being perpetuated via powerful physical and social boundaries. It had to be continually maintained, and was regularly challenged by Greenwich's occupants and neighbours.

9.
New Phytol ; 224(1): 146-154, 2019 10.
Artículo en Inglés | MEDLINE | ID: mdl-31211874

RESUMEN

Growing evidence indicates that tree-stem methane (CH4 ) emissions may be an important and unaccounted-for component of local, regional and global carbon (C) budgets. Studies to date have focused on upland and freshwater swamp-forests; however, no data on tree-stem fluxes from estuarine species currently exist. Here we provide the first-ever mangrove tree-stem CH4 flux measurements from  >50 trees (n = 230 measurements), in both standing dead and living forest, from a region suffering a recent large-scale climate-driven dieback event (Gulf of Carpentaria, Australia). Average CH4 emissions from standing dead mangrove tree-stems was 249.2 ± 41.0 µmol m-2  d-1 and was eight-fold higher than from living mangrove tree-stems (37.5 ± 5.8 µmol m-2  d-1 ). The average CH4 flux from tree-stem bases (c. 10 cm aboveground) was 1071.1 ± 210.4 and 96.8 ± 27.7 µmol m-2  d-1 from dead and living stands respectively. Sediment CH4 fluxes and redox potentials did not differ significantly between living and dead stands. Our results suggest both dead and living tree-stems act as CH4 conduits to the atmosphere, bypassing potential sedimentary oxidation processes. Although large uncertainties exist when upscaling data from small-scale temporal measurements, we estimated that dead mangrove tree-stem emissions may account for c. 26% of the net ecosystem CH4 flux.


Asunto(s)
Avicennia/metabolismo , Carbono/metabolismo , Bosques , Metano/metabolismo , Tallos de la Planta/metabolismo , Geografía , Sedimentos Geológicos/química , Oxidación-Reducción , Queensland , Volatilización
10.
Environ Sci Technol ; 53(11): 6420-6426, 2019 06 04.
Artículo en Inglés | MEDLINE | ID: mdl-31117543

RESUMEN

Atmospheric concentrations of methane have increased ∼2.4 fold since the industrial revolution with wetlands and inland waters representing the largest source of methane to the atmosphere. Substantial uncertainties remain in global methane budgets, due in part to the lack of adequate techniques and detailed measurements to assess ebullition in aquatic environments. Here, we present details of a low cost (∼$120 US per unit) ebullition sensor that autonomously logs both volumetric ebullition rate and methane concentrations. The sensor combines a traditional funnel bubble trap with an Arduino logger, a pressure sensor, thermal conductivity methane sensor, and a solenoid valve. Powered by three AA batteries, the sensor can measure autonomously for three months when programmed for a sampling frequency of 30 min. For field testing, four sensors were deployed for six weeks in a small lake. While ebullition was spatially and temporally variable, a distinct diurnal trend was observed with the highest rates from mid-morning to early afternoon. Ebullition rates were similar for all four sensors when integrated over the sampling period. The widespread deployment of low cost automated ebullition sensors such as the iAMES described here will help constrain one of the largest uncertainties in the global methane budget.


Asunto(s)
Atmósfera , Metano , Lagos
11.
Environ Sci Technol ; 52(3): 1118-1127, 2018 02 06.
Artículo en Inglés | MEDLINE | ID: mdl-29303570

RESUMEN

Antimony (Sb) and arsenic (As) are priority environmental contaminants that often co-occur at mining-impacted sites. Despite their chemical similarities, Sb mobility in waterlogged sediments is poorly understood in comparison to As, particularly across the sediment-water interface (SWI) where changes can occur at the millimeter scale. Combined diffusive gradients in thin films (DGT) and diffusive equilibration in thin films (DET) techniques provided a high resolution, in situ comparison between Sb, As, and iron (Fe) speciation and mobility across the SWI in contaminated freshwater wetland sediment mesocosms under an oxic-anoxic-oxic transition. The shift to anoxic conditions released Fe(II), As(III), and As(V) from the sediment to the water column, consistent with As release being coupled to the reductive dissolution of iron(III) (hydr)oxides. Conversely, Sb(III) and Sb(V) effluxed to the water column under oxic conditions and fluxed into the sediment under anoxic conditions. Porewater DGT-DET depth profiles showed apparent decoupling between Fe(II) and Sb release, as Sb was primarily mobilized across the SWI under oxic conditions. Solid-phase X-ray absorption spectroscopy (XAS) revealed the presence of an Sb(III)-S phase in the sediment that increased in proportion with depth and the transition from oxic to anoxic conditions. The results of this study showed that Sb mobilization was decoupled from the Fe cycle and was, therefore, more likely linked to sulfur and/or organic carbon (e.g., most likely authigenic antimony sulfide formation or Sb(III) complexation by reduced organic sulfur functional groups).


Asunto(s)
Arsénico , Antimonio , Compuestos Férricos , Sedimentos Geológicos , Humedales
13.
Environ Sci Technol ; 51(17): 9739-9746, 2017 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-28766328

RESUMEN

Schwertmannite is a ferric oxyhydroxysulfate mineral, which is common in acid sulfate systems. Such systems contain varying concentrations of phosphate (PO43-)-an essential nutrient whose availability may be coupled to schwertmannite formation and fate. This study examines the effect of phosphate on schwertmannite stability under reducing conditions. Phosphate was added at 0, 80, 400, and 800 µmoles g-1 (i.e., zero, low, medium, and high loading) to schwertmannite suspensions which were inoculated with wetland sediment and suspended in N2-purged artificial groundwater. pH remained between 2.7 and 4.3 over the 41 day experiment duration. Fe(II) accumulated in solution due to dissimilatory Fe(III)-reduction, which was most pronounced at intermediate PO43- loadings (i.e., in the low PO43- treatment). Partial transformation of schwertmannite to goethite occurred in the zero and low PO43- treatments, with negligible transformation in higher PO43- treatments. Overall, the results suggest that intermediate PO43- loadings provide conditions which facilitate optimal reductive dissolution of schwertmannite. At zero PO43- loading, reductive dissolution appears to be constrained by the rapid transformation of schwertmannite to goethite, which thereby decreases the bioavailability of solid-phase Fe(III). Conversely, at high loadings, PO43- appears to stabilize the schwertmannite surface against dissolution; probably via the formation of strong surface complexes.


Asunto(s)
Compuestos de Hierro/química , Fosfatos/química , Arsénico , Disponibilidad Biológica , Compuestos Férricos , Oxidación-Reducción
14.
Environ Sci Technol ; 51(8): 4259-4268, 2017 04 18.
Artículo en Inglés | MEDLINE | ID: mdl-28347133

RESUMEN

Jarosite can be an important scavenger for arsenic (As) and antimony (Sb) in acid mine drainage (AMD) and acid sulfate soil (ASS) environments. When subjected to reducing conditions, jarosite may undergo reductive dissolution, thereby releasing As, Sb, and Fe2+ coincident with a rise in pH. These conditions can also trigger the Fe2+-induced transformation of jarosite to more stable Fe(III) minerals, such as goethite. However, the consequences of this transformation process for As and Sb are yet to be methodically examined. We explore the effects of abiotic Fe2+-induced transformation of jarosite on the mobility, speciation, and partitioning of associated As(V) and Sb(V) under anoxic conditions at pH 7. High concentrations of Fe2+ (10 and 20 mM) rapidly (<10 min) transformed jarosite to a green rust intermediary, prior to the subsequent precipitation of goethite within 24 h. In contrast, lower concentrations of Fe2+ (1 and 5 mM) led to the formation of lepidocrocite. As K-edge XANES spectroscopy revealed some reduction of As(V) to As(III) at higher concentrations of Fe2+, while Sb L1-edge XANES spectroscopy indicated no reduction of Sb(V). The transformation processes enhanced Sb mobilization into the aqueous phase, while As was instead repartitioned to a surface-bound exchangeable phase. The results imply that Fe2+-induced transformation of As/Sb-jarosite can increase Sb mobility and exert major influences on As partitioning and speciation.


Asunto(s)
Arsénico , Compuestos Férricos/química , Antimonio/química , Compuestos Ferrosos/química , Minería , Oxidación-Reducción
15.
Phys Rev Lett ; 117(6): 067601, 2016 Aug 05.
Artículo en Inglés | MEDLINE | ID: mdl-27541475

RESUMEN

Many chalcogenide glasses undergo a breakdown in electronic resistance above a critical field strength. Known as threshold switching, this mechanism enables field-induced crystallization in emerging phase-change memory. Purely electronic as well as crystal nucleation assisted models have been employed to explain the electronic breakdown. Here, picosecond electric pulses are used to excite amorphous Ag_{4}In_{3}Sb_{67}Te_{26}. Field-dependent reversible changes in conductivity and pulse-driven crystallization are observed. The present results show that threshold switching can take place within the electric pulse on subpicosecond time scales-faster than crystals can nucleate. This supports purely electronic models of threshold switching and reveals potential applications as an ultrafast electronic switch.

16.
Environ Sci Technol ; 50(15): 8010-9, 2016 08 02.
Artículo en Inglés | MEDLINE | ID: mdl-27403840

RESUMEN

Fires in iron-rich seasonal wetlands can thermally transform Fe(III) minerals and alter their crystallinity. However, the fate of As associated with thermally transformed Fe(III) minerals is unclear, as are the consequences for As mobilization during subsequent reflooding and reductive cycles. Here, we subject As(V)-coprecipitated schwertmannite to thermal transformation (200, 400, 600 and 800 °C) followed by biotic reductive incubation (150 d) and examine aqueous- and solid-phase speciation of As, Fe and S. Heating to >400 °C caused transformation of schwertmannite to a nanocrystalline hematite with greater surface area and smaller particle size. Higher temperatures also caused the initially structurally incorporated As to become progressively more exchangeable, increasing surface-complexed As (AsEx) by up to 60-fold, thereby triggering enhanced As mobilization during incubation (∼70-fold in the 800 °C treatment). Although more As was mobilized in biotic treatments than controls (∼3-20×), in both cases it was directly proportional to initial AsEx and mainly due to abiotic desorption. Higher transformation temperatures also drove divergent pathways of Fe and S biomineralization and led to more As(V) and SO4 reduction relative to Fe(III) reduction. This study reveals thermal transformation of schwertmannite can greatly increase As mobility and has major consequences for As/Fe/S speciation under reducing conditions. Further research is warranted to unravel the wider implications for water quality in natural wetlands.


Asunto(s)
Arsénico , Compuestos Férricos , Hierro/química , Oxidación-Reducción , Contaminantes Químicos del Agua
17.
J Trauma Stress ; 28(6): 499-504, 2015 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-26595460

RESUMEN

Military personnel deployed to Joint Task Force Guantanamo Bay (JTF-GTMO) faced numerous occupational stressors. As part of a program evaluation, personnel working at JTF-GTMO completed several validated self-report measures. Personnel were at the beginning, middle, or end of their deployment phase. This study presents data regarding symptoms of posttraumatic stress disorder, alcohol abuse, depression, and resilience among 498 U.S. military personnel deployed to JTF-GTMO in 2009. We also investigated individual and organizational correlates of mental health among these personnel. Findings indicated that tenure at JTF-GTMO was positively related to adverse mental health outcomes. Regression models including these variables had R2 values ranging from .02 to .11. Occupation at JTF-GTMO also related to mental health such that guards reported poorer mental health than medical staff. Reluctance to seek out mental health care was also related to mental health outcomes. Those who reported being most reluctant to seek out care tended to report poorer mental health than those who were more willing to seek out care. Results suggested that the JTF-GTMO deployment was associated with significant psychological stress, and that both job-related and attitude-related variables were important to understanding mental health symptoms in this sample.


Asunto(s)
Servicios de Salud Mental/normas , Salud Mental , Personal Militar/psicología , Enfermedades Profesionales/psicología , Aceptación de la Atención de Salud/psicología , Prisiones , Trastornos por Estrés Postraumático/psicología , Adolescente , Adulto , Análisis de Varianza , Actitud Frente a la Salud , Trastorno Depresivo/diagnóstico , Femenino , Humanos , Masculino , Servicios de Salud Mental/provisión & distribución , Enfermedades Profesionales/etiología , Aceptación de la Atención de Salud/estadística & datos numéricos , Prisiones/organización & administración , Análisis de Regresión , Estudios Retrospectivos , Trastornos por Estrés Postraumático/diagnóstico , Trastornos por Estrés Postraumático/etiología , Encuestas y Cuestionarios , Estados Unidos , Recursos Humanos , Adulto Joven
18.
Environ Sci Technol ; 48(23): 13660-7, 2014 Dec 02.
Artículo en Inglés | MEDLINE | ID: mdl-25346449

RESUMEN

In floodplain soils, As may be released during flooding-induced soil anoxia, with the degree of mobilization being affected by microbial redox processes such as the reduction of As(V), Fe(III), and SO4(2-). Microbial SO4(2-) reduction may affect both Fe and As cycling, but the processes involved and their ultimate consequences on As mobility are not well understood. Here, we examine the effect of microbial SO4(2) reduction on solution dynamics and solid-phase speciation of As during flooding of an As-contaminated soil. In the absence of significant levels of microbial SO4(2-) reduction, flooding caused increased Fe(II) and As(III) concentrations over a 10 week period, which is consistent with microbial Fe(III)- and As(V)-reduction. Microbial SO4(2-) reduction leads to lower concentrations of porewater Fe(II) as a result of FeS formation. Scanning electron microscopy with energy dispersive X-ray fluorescence spectroscopy revealed that the newly formed FeS sequestered substantial amounts of As. Bulk and microfocused As K-edge X-ray absorption near-edge structure spectroscopy confirmed that As(V) was reduced to As(III) and showed that in the presence of FeS, solid-phase As was retained partly via the formation of an As2S3-like species. High resolution transmission electron microscopy suggested that this was due to As retention as an As2S3-like complex associated with mackinawite (tetragonal FeS) rather than as a discrete As2S3 phase. This study shows that mackinawite formation in contaminated floodplain soil can help mitigate the extent of arsenic mobilization during prolonged flooding.


Asunto(s)
Arsénico/análisis , Inundaciones , Hierro/análisis , Microbiología del Suelo , Contaminantes del Suelo/análisis , Sulfatos/metabolismo , Arsénico/química , Australia , Compuestos Ferrosos/química , Hierro/química , Oxidación-Reducción , Contaminantes del Suelo/química , Soluciones , Espectrometría por Rayos X/métodos , Sulfatos/química , Espectroscopía de Absorción de Rayos X
19.
J Hazard Mater ; 476: 135013, 2024 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-38925052

RESUMEN

Arsenic (As) and antimony (Sb) often co-occur in floodplain depositional environments that are contaminated by legacy mining activities. However, the distribution of As and Sb throughout floodplains is not uniform, adding complexity and expense to management or remediation processes. Identifying floodplain morphology predictor variables that help quantify and explain As and Sb spatial distribution on floodplains is useful for management and remediation. We developed As and Sb risk maps estimating concentration and availability at a coastal floodplain wetland impacted by upper-catchment mining. Significant predictors of As and Sb concentrations included i) distance from distributary channel-wetland intersection and ii) elevation. Distance from channel explained 53 % (P < 0.01) and 28 % (P < 0.01), while elevation explained 42 % (P < 0.01) and 47 % (P < 0.01) of the variability in near-total Sb and As respectively. As had a higher extractability than Sb across all tested soil extractions, suggesting that As is more environmentally available. As and Sb dry mass estimates to a depth of 0.1 m scaled to the lower coastal Macleay floodplain ranged from 113-192 tonnes and 14-24 tonnes respectively. Landscape-scale modelling of metalloid distribution, informed by morphology variables, presented here may be a useful framework for the development of risk maps in other regions impacted by contaminated upper-catchment sediments.

20.
Sci Total Environ ; 935: 173345, 2024 Jul 20.
Artículo en Inglés | MEDLINE | ID: mdl-38782265

RESUMEN

Intermittently closed and open coastal lakes and lagoons (ICOLLs) are ecologically important and hydrologically sensitive estuarine systems. We explore how extreme drought and ICOLL entrance management intersect to influence the geochemical cycling of iron. Opening the ICOLL entrance just prior to an extreme drought in 2019 led to prolonged extremely low water levels, thereby exposing intertidal/subtidal sulfidic sediments and causing oxidation of sedimentary pyrite. Subsequent reflooding of exposed sediments for ∼4 months led to extremely elevated Fe2+(aq) (>10 mM) in intertidal hyporheic porewaters, consistent with Fe2+(aq) release via pyrite oxidation and via reductive dissolution of newly-formed Fe(III) phases. Re-opening the ICOLL entrance caused a rapid fall in water levels (∼1.5 m over 7 d), driving the development of effluent groundwater gradients in the intertidal zone, thereby transporting Fe2+-rich porewater into surface sediments and surface waters. This was accompanied by co-mobilisation of some trace metals and nutrients. On contact with oxic, circumneutral-pH estuarine water, the abundant Fe2+(aq) oxidised, forming a spatially extensive accumulation of poorly crystalline Fe(III) oxyhydroxide floc (up to 25 % Fe dry weight) in shallow intertidal zone benthic sediments throughout the ICOLL. Modelling estimates ∼4050 × 103 kg of poorly-crystalline Fe was translocated into surficial sediments. The newly formed Fe(III)-oxyhydroxides serve as a metastable sink encouraging enrichment of both phosphate and various trace metal(loid)s in near-surface sediments, which may have consequences for future cycling of nutrients, metals and ICOLL ecological function. The additional Fe also may enhance ICOLL sensitivity to similar future drought events by encouraging pyrite formation in shallow (<5 cm) benthic sediments. This system-wide translocation of Fe from deeper sediments into surficial benthic sediments represents a form of geochemical hysteresis with an uncertain recovery trajectory. This study demonstrates how climate extremes can interact with anthropogenic management to amplify ICOLL hydrological oscillations and influence biogeochemistry in complex ways.

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