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1.
Sci Total Environ ; 951: 175082, 2024 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-39097030

RESUMEN

Lake Naivasha, Kenya's second-largest freshwater body is a wetland of international ecological importance and currently subjected to unprecedented anthropogenic influence. The study aims to chronologically reconstruct the main human activities and background weathering reactions that govern metal mobilizations into the lake and their potentially adverse effects on its ecological status. We combine extensive geochemical analyses (major, trace elements, Zn-Pb isotope ratios) in a dated lake sediment record and catchment rocks with remote sensing techniques. Downcore geochemical variations reflect natural ecosystem destabilizations occurring as early as the first half of the 20th century. These coincide with changes towards less radiogenic Pb-isotope values which persist towards the top of the core (206Pb/207Pb = 1.243 at core base ∼1843, to 206Pb/207Pb = 1.225 at ∼1978). We interpret the land-clearance for agricultural purposes on the Aberdare Range and documented early aviation activities as possible vectors of this early Pb-isotope excursion. The overlapping Pb-isotope signatures between sediment sources and anthropogenic contributions challenges a straightforward deconvolution of the two. Our conservative model calculations suggest, nevertheless, that an addition of up to ∼1.8 % Pb-gasoline influx to the total Pb flux, peaking in the 1980s is able to explain the Pb distribution trend. Homogeneous Zn-isotope compositions in sediments deposited until ∼1970s (δ66/64Zn = 0.216-0.225 ‰) do not follow major hydro-climatic events or anthropogenic forcing but likely reflect lake-specific natural cycling. Subsequent higher variations to both heavier (up to δ66/64Zn = 0.242 ± 0.005 ‰) and lighter (down to δ66/64Zn = 0.184 ± 0.003 ‰) Zn-isotope values are contemporaneous with intensification of large-scale horticultural industry in the catchment. Together with supporting indicators, the lighter Zn-isotope compositions in youngest analysed sediments (21st century) are attributable to increased biological productivity (algal blooms) and ongoing lake eutrophication. Our study demonstrates the applicability of the heavy metal isotope tool to reconstruct human influences on lake environments with complex geological settings such as the East African Rift System.


Asunto(s)
Monitoreo del Ambiente , Lagos , Oligoelementos , Contaminantes Químicos del Agua , Lagos/química , Kenia , Contaminantes Químicos del Agua/análisis , Oligoelementos/análisis , Sedimentos Geológicos/química , Metales/análisis , Isótopos/análisis
2.
Environ Geochem Health ; 46(10): 395, 2024 Aug 24.
Artículo en Inglés | MEDLINE | ID: mdl-39180633

RESUMEN

Dispersion of potentially toxic elements associated with efflorescent crusts and mine tailings materials from historical mine sites threaten the environment and human health. Limited research has been done on traceability from historical mining sites in arid and semi-arid regions. Pb isotope systematics was applied to decipher the importance of identifying the mixing of lead sources involved in forming efflorescent salts and the repercussions on traceability. This research assessed mine waste (sulfide-rich and oxide-rich tailings material and efflorescent salts) and street dust from surrounding settlements at a historical mining site in northwestern Mexico, focusing on Pb isotope composition. The isotope data of tailings materials defined a trending line (R2 = 0.9); the sulfide-rich tailings materials and respective efflorescent salts yielded less radiogenic Pb composition, whereas the oxide-rich tailings and respective efflorescent salts yielded relatively more radiogenic compositions, similar to the geogenic component. The isotope composition of street dust suggests the dispersion of tailings materials into the surroundings. This investigation found that the variability of Pb isotope composition in tailings materials because of the geochemical heterogeneity, ranging from less radiogenic to more radiogenic, can add complexity during environmental assessments because the composition of oxidized materials and efflorescent salts can mask the geogenic component, potentially underestimating the influence on the environmental media.


Asunto(s)
Polvo , Isótopos , Plomo , Minería , Plomo/análisis , Isótopos/análisis , Polvo/análisis , México , Monitoreo del Ambiente , Contaminantes del Suelo/análisis
3.
Mar Pollut Bull ; 204: 116534, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38850759

RESUMEN

Marinas are central hubs of global maritime leisure and transport, yet their operations can deteriorate the environmental quality of sediments. In response, this study investigated the metal contamination history associated with antifouling paint uses in a sediment core collected from Bracuhy marina (Southeast Brazil). Analysis target major and trace elements (Cu, Zn, Pb, Cd and Sn), rare earth elements (REEs), and Pb isotopes. The modification in Pb isotopic ratios and REEs pattern unequivocally revealed sediment provenance disruption following the marina construction. Metal distribution in the sediment core demonstrates that concentrations of Cu and Zn increased by up to 15 and 5 times, respectively, compared to the local background. This severe Cu and Zn contamination coincides with the onset of marina operations and can be attributed to the use of antifouling paints.


Asunto(s)
Cobre , Monitoreo del Ambiente , Sedimentos Geológicos , Pintura , Contaminantes Químicos del Agua , Sedimentos Geológicos/química , Pintura/análisis , Contaminantes Químicos del Agua/análisis , Cobre/análisis , Brasil , Navíos
4.
Environ Geochem Health ; 46(5): 164, 2024 Apr 09.
Artículo en Inglés | MEDLINE | ID: mdl-38592563

RESUMEN

Lead (Pb) poses a significant risk to infants and children through exposure to contaminated soil and dust. However, there is a lack of information on Pb speciation and distribution at the neighborhood-scale. This work aimed to determine: (1) the distribution of acid-extractable (labile) Pb and other metals ([M]AE) in two neighborhoods in Akron, Ohio (USA) (Summit Lake and West Akron; n = 82 samples); and (2) Pb speciation and potential sources. Total metal concentration ([M]T) and [M]AE was strongly correlated for Pb and Zn (R2 of 0.66 and 0.55, respectively), corresponding to 35% and 33% acid-extractability. Lead and Zn exhibited a strong positive correlation with each other (R2 = 0.56 for MT and 0.68 for MAE). Three types of Pb-bearing phases were observed by electron microscopy: (1) galena (PbS)-like (5-10 µm); (2) paint chip residuals (10-20 µm); and (3) Pb-bearing Fe-oxides (20 µm). Isotope ratio values for PbAE were 1.159 to 1.245 for 206Pb/207Pb, and 1.999 to 2.098 for 208Pb/206Pb, and there was a statistically significant difference between the two neighborhoods (p = 0.010 for 206Pb/207Pb and p = 0.009 for 208Pb/206Pb). Paint and petrol are the dominant sources of Pb, with some from coal and fly ash. Lead speciation and distribution is variable and reflects a complex relationship between the input of primary sources and post-deposition transformations. This work highlights the importance of community science collaborations to expand the reach of soil sampling and establish areas most at risk based on neighborhood-dependent Pb speciation and distribution for targeted remediation.


Asunto(s)
Carbón Mineral , Suelo , Niño , Lactante , Humanos , Ohio , Ceniza del Carbón , Polvo
5.
J Hazard Mater ; 466: 133568, 2024 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-38262321

RESUMEN

Facility agriculture enhances food production capabilities. However, concerns persist regarding heavy metal accumulation resulting from extensive operation of this type of farming. This study integrated the total content, five fractions, and isotope composition of Cd and Pb in intensively farmed soils in regions characterized by industrialization (Shaoguan, SG) and urbanization (Guangzhou, GZ), to assess the sources and mechanisms causing metals accumulation. We found significantly more severe Cd/Pb accumulation and potential mobility in SG than GZ. Cd displayed higher accumulation levels and potential mobility than Pb. The distinct isotopic signals in SG (-0.54 to 0.47‰ for δ114/110Cd and 1.1755 to 1.1867 for 206Pb/207Pb) and GZ (-0.86 to 0.12‰ for δ114/110Cd and 1.1914 to 1.2012 for 206Pb/207Pb) indicated significant differences in Cd/Pb sources. The Bayesian model revealed that industrial activities and related transportation accounted for over 40% and approximately 30%, respectively, of the average contributions of Cd/Pb in SG. While urban-related (26.6%) and agricultural-related (26.3%) activities primarily contributed to Cd in GZ. The integration of δ114/110Cd and 208Pb/206Pb has further enhanced the regional contrast in sources. The present study established a comprehensive tracing system for Cd-Pb, providing crucial insights into the accumulation and distribution of these metals in facility agricultural soils.

6.
Mar Environ Res ; 191: 106129, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37586223

RESUMEN

The Bering Sea and the Chukchi Sea are important regions for marine ecosystems and climate change. However, the historical deposition and sources of metals in these regions are poorly understood. In this study, we utilized Pb isotopes and multi-element concentrations (Ni, Cu, Fe, Mn, Zn, Cd, Pb) coupled with Pb-210 dating to investigate the historical deposition and source identification of metals in sediment cores collected from the Bering Sea and the Chukchi Sea. Our findings reveal that the transport of organic matter was mainly transported by marine and terrestrial sources in the Bering and Chukchi Sea, respectively. Historical variations of metals were similar in both seas, showing an increasing trend of metals (excluding Mn) from the 1960s to the 1990s, followed by a gradual decrease after the 1990s, which can be attributed to the development of industrial and gasoline emission. The results of the geo-accumulation index indicated that sediment in both seas was relatively unpolluted with metals. Additionally, Pb isotopic ratios suggested that natural weathering was the primary source of Pb in the area, but the use and phase-out of gasoline were also well-reconstructed. This study provides valuable information for assessing environmental changes and human activities over the past century in the Arctic and subarctic Ocean.


Asunto(s)
Metales Pesados , Contaminantes Químicos del Agua , Humanos , Plomo , Sedimentos Geológicos , Gasolina , Ecosistema , Contaminantes Químicos del Agua/análisis , Monitoreo del Ambiente/métodos , Océanos y Mares , Metales Pesados/análisis , Actividades Humanas
7.
Environ Sci Pollut Res Int ; 30(38): 89442-89458, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37453008

RESUMEN

The accumulation, pathways, and sources of anthropogenic lead (Pb) in Ulleung Basin sediments were investigated based on the temporal and spatial variations in the Pb concentration and stable Pb isotopes for 21 dated box core sediments collected from the shelf, slope, and basin in the southern East/Japan Sea. Leached (1 M HCl) Pb concentrations and isotope ratios (207Pb/206Pb and 208Pb/206Pb) were nearly constant before 1930, but have increased rapidly until the present. The primary source of anthropogenic Pb is considered to be atmospheric deposition, showing the signature of a mixture of leaded gasoline and coals, which was the major anthropogenic source in the basin. However, after the 1990s, anthropogenic Pb from dumping materials added as much as 10-25% to the slope sediment and has been spreading out from the water column accompanied by the movement of the East Sea Intermediate Water. In shelf areas, inputs from nonferrous refineries in the coastal industrial complexes play an important role in pollution from anthropogenic Pb.


Asunto(s)
Contaminantes Químicos del Agua , Contaminantes Químicos del Agua/análisis , Plomo , Sedimentos Geológicos , Japón , Monitoreo del Ambiente , Isótopos/análisis , Agua
8.
Proc Natl Acad Sci U S A ; 120(23): e2219688120, 2023 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-37252961

RESUMEN

Reversible scavenging, the oceanographic process by which dissolved metals exchange onto and off sinking particles and are thereby transported to deeper depths, has been well established for the metal thorium for decades. Reversible scavenging both deepens the elemental distribution of adsorptive elements and shortens their oceanic residence times in the ocean compared to nonadsorptive metals, and scavenging ultimately removes elements from the ocean via sedimentation. Thus, it is important to understand which metals undergo reversible scavenging and under what conditions. Recently, reversible scavenging has been invoked in global biogeochemical models of a range of metals including lead, iron, copper, and zinc to fit modeled data to observations of oceanic dissolved metal distributions. Nonetheless, the effects of reversible scavenging remain difficult to visualize in ocean sections of dissolved metals and to distinguish from other processes such as biological regeneration. Here, we show that particle-rich "veils" descending from high-productivity zones in the equatorial and North Pacific provide idealized illustrations of reversible scavenging of dissolved lead (Pb). A meridional section of dissolved Pb isotope ratios across the central Pacific shows that where particle concentrations are sufficiently high, such as within particle veils, vertical transport of anthropogenic surface-dissolved Pb isotope ratios toward the deep ocean is manifested as columnar isotope anomalies. Modeling of this effect shows that reversible scavenging within particle-rich waters allows anthropogenic Pb isotope ratios from the surface to penetrate ancient deep waters on timescales sufficiently rapid to overcome horizontal mixing of deep water Pb isotope ratios along abyssal isopycnals.

9.
Environ Pollut ; 330: 121740, 2023 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-37121303

RESUMEN

Atmospheric deposition is an essential pathway of heavy metals (HMs) from the atmosphere to soils, while few studies assess the effects and contributions of atmospheric deposition on HMs accumulations in agricultural soils from the field and regional scales. In this study, eleven representative field monitoring sites from industrial areas, agricultural areas, and reference site in a typical rapid industrial development region were selected to determine the effects of atmospheric deposition on soil HMs accumulation. Industrial activities significantly increased the deposited particles flux from atmospheric deposition, with annual particles fluxes in industrial areas being 1.83 and 1.90 times higher than in agricultural areas and reference site, respectively. Although the HMs deposition fluxes had decreased significantly with time by literature comparison, the deposition fluxes of Cd and Pb were still at high levels in this study area. Precipitation was the key factor affecting seasonal variations of atmospheric HMs deposition. Lead isotope analysis indicated that atmospheric Pb originated from coal combustion, and atmospheric deposition was the primary source of Pb contamination in agricultural soil adjacent to industries. This study provided insight into the effects of atmospheric deposition on agricultural soil HMs accumulations at the regional scale and an important theoretical basis for source-preventing soil HMs contamination in industrial developed and other similar areas.


Asunto(s)
Metales Pesados , Contaminantes del Suelo , Suelo , Plomo/análisis , Monitoreo del Ambiente , Contaminantes del Suelo/análisis , Metales Pesados/análisis , Isótopos/análisis , China , Medición de Riesgo
10.
Sci Total Environ ; 871: 162067, 2023 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-36758690

RESUMEN

Millions of lead (Pb) pipes are still used in the drinking water distribution systems in many regions in the world. Human exposure to Pb from contaminated drinking water continues to be of concern in the United States (U.S.), as illustrated by the widely publicized "Flint Water Crisis" in 2015. The Pb isotopic composition of Pb-pipes potentially can be useful to identify human exposure to Pb from lead service lines (LSLs). In addition, as the LSLs were likely manufactured from similar industrial Pb sources as other Pb objects and materials in the USA, the Pb-pipes isotope data can provide information about the overall isotopic composition of the U.S. industrial Pb. In this work we present high-precision Pb isotope data from Pb-pipes excavated from different U.S. municipalities. The Pb-pipes show an extremely wide range of Pb isotopic compositions, with 206Pb/204Pb ranging from 17.004 to 22.010, 207Pb/204Pb from 15.460 to 15.921, and 208Pb/204Pb from 36.687 to 41.120. The wide isotope range is observed even in a single town, suggesting that no regional Pb isotope patterns can be expected within the continental USA. However, the high-precision MC-ICP-MS Pb data form a clear linear trend that, depending on the context, can be used to identify human Pb exposure. Furthermore, as the linear trend is a result of utilization of Pb ores from different domestic and international sources and secondary recycling of metallic Pb, it is likely representative of the overall isotopic composition of the U.S. industrial Pb pool. Therefore, the identified trend is the most accurate isotope representation of the U.S. anthropogenic Pb at present and can be used as first-order evaluation to determine if a person with elevated blood Pb levels was exposed to U.S. industrial Pb sources.


Asunto(s)
Agua Potable , Humanos , Estados Unidos , Plomo , Ciudades , Isótopos/análisis , Industrias , Monitoreo del Ambiente
11.
J Hazard Mater ; 448: 130828, 2023 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-36731315

RESUMEN

In 2019, the Brumadinho dam rupture released a massive amount of iron ore mining tailings into the Paraopeba River. Up to now, it remains a public health issue for the local and downstream populations. The present study aims to assess the behavior and fate of metal contamination following the disaster. Using new sampling strategies and up-to-date geochemistry tools, we show that the dissolved metal concentrations (< 0.22 µm cutoff filtration) remained low in the Paraopeba River. Although the tailings present high metal concentrations (Fe, Mn, Cd, and As), the high local background contents of metals and other previous anthropogenic contamination hamper tracing the sediment source based only on the geochemical signature. The Pb isotopic composition coupled with the metals enrichment factor of sediments and Suspended Particulate Matter (SPM) constitutes accurate proxies that trace the fate and dispersion of tailing particles downstream of the dam collapse. This approach shows that 1) The influence of the released tailing was restricted to the Paraopeba River and the Retiro Baixo reservoir, located upstream of the São Francisco River; 2) The tailings' contribution to particulate load ranged from 17 % to 88 % in the Paraopeba River; 3) Other regional anthropogenic activities also contribute to water and sediment contamination of the Paraopeba river.

12.
Chemosphere ; 322: 138169, 2023 May.
Artículo en Inglés | MEDLINE | ID: mdl-36812994

RESUMEN

Clarifying the sources and historical variation of metal(loid)s in agricultural river sediments is vital for watershed contamination control and environmental improvements. In this study, a systematical geochemical investigation of Pb isotopic characteristics and the spatial-temporal distribution of metal(loid)s abundances was conducted to delineate the origins of metal(loid)s (Cd, Zn, Cu, Pb, Cr, and As) in sediments from an agricultural river, Sichuan Province, Southwest China. The results showed significant enrichment of Cd and Zn in the whole watershed, with substantial anthropogenic contributions of 86.1% and 63.1% for the surface sediments, and 79.1% and 67.9% for the core sediments, respectively. As was mainly derived from natural sources. Cu, Cr, and Pb were originated from the mixing sources of natural and anthropogenic processes. The anthropogenic origin of Cd, Zn, and Cu in the watershed was closely correlated with agricultural activities. The profile of EF-Cd and EF-Zn displayed an increasing trend from the 1960s-1990s, and then kept a high value, which was consistent with the development of national agricultural activities. Pb isotopic signatures suggested multiple sources of the anthropogenic Pb contamination, including industrial/sewage discharge, coal combustion, and vehicle exhaust. The average anthropogenic 206Pb/207Pb ratio (1.1585) approximated that of local aerosols (1.1660), suggesting aerosol deposition was a crucial pathway of anthropogenic Pb input to sediment. Furthermore, the anthropogenic Pb percentages (mean of 52.3 ± 10.3%) from the EF approach were in line with that from the Pb isotopic method (mean of 45.5 ± 13.3%) for sediments under intense anthropogenic impacts.


Asunto(s)
Metales Pesados , Contaminantes Químicos del Agua , Plomo/análisis , Cadmio/análisis , Ríos , Monitoreo del Ambiente , Sedimentos Geológicos , China , Isótopos/análisis , Metales Pesados/análisis , Contaminantes Químicos del Agua/análisis , Medición de Riesgo
13.
Sci Total Environ ; 867: 161405, 2023 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-36621473

RESUMEN

Extensive mining and smelting contributed to the declining quality of Luanshya soils. The local smelter was the epicenter of contamination as shown by a spatial distribution analysis. Closeby soil profiles smelter exhibit extremely high Cu concentrations (up to 46,000 mg kg-1 Cu) relative to deeper layers where only background levels of trace elements were observed. A remote profile did not exhibit significant contamination. Lead isotopic ratios revealed that Pb contamination in the Luanshya soils was not smelter-derived. It was shown in this way that the historical usage of leaded gasoline was the main source of this metal. Although the Luanshya smelter also produced Co, this metal was not an important contaminant. Copper leaching was a concern in Luanshya. Upwards of 52 % of Cu was extractable in the exchangeable step of a sequential extraction procedure (SEP), but only for samples where Cu concentrations were high, suggesting that Cu was released exclusively from anthropogenic particles. This was supported by the SEP results for similar depths at the remote soil, where only a small fraction of Cu was labile (5.6 %). Lead and Co were strongly bound in the soils throughout. The excess of Cu in the topsoils was mostly bound in smelter-derived particles. These appeared as spherical fast-cooled droplets composed mostly of sulfides, oxides, and glass. X-ray diffraction and electron probe microanalysis of those particles allowed for a phase classification. Compositions were regularly not stoichiometric so most particles were classified as intermediate solid solutions. However, molecular proportions often closely resembled those of bornite, chalcanthite, cuprospinel, covellite, delafossite, diginite, or hydrous ferric oxides. Concentrations of Cu were often 100 % near the center of the particles indicating an inefficient smelting process. Weathering to some degree was common, which in conjunction with the susceptibility of Cu leaching was highly alarming.

14.
Environ Pollut ; 320: 121097, 2023 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-36657515

RESUMEN

Heavy metal pollutants resulting from human activities consistently move from the topsoil to the subsoil profiles under the influence of rainfall leaching. This study intends to predict the long-term transport of heavy metals at an abandoned e-waste recycling site with respect to historical pollution activities, land use, and metal pollutant dynamics. Our results showed that the site was seriously contaminated with heavy metals (Cd, Cu, Pb, and Zn) in the soil profiles. More specifically, Cu and Zn accumulated primarily in the upper layers of the soil profile owing to their weak mobility, while significant migration of Cd and Pb was observed in the deeper soil layers. Furthermore, to clarify the fate of Pb in soil profiles, Pb isotopes and the Hydrus model were used to trace the sources of Pb contamination and predict its long-term distribution. The Pb isotope results suggest that past e-waste recycling activities significantly contributed to the heavy metal concentration in the soil profiles; however, other anthropogenic sources such as vehicle exhaust had smaller impacts. Moreover, our model findings predicted that within the next 30 years, 60% of Pb contaminants will be concentrated in the surface soil. Together these results provide a theoretical foundation and scientific basis for evaluating, controlling, and remediating abandoned e-waste recycling sites.


Asunto(s)
Residuos Electrónicos , Contaminantes Ambientales , Metales Pesados , Contaminantes del Suelo , Humanos , Suelo , Cadmio , Plomo , Contaminantes del Suelo/análisis , Monitoreo del Ambiente/métodos , Metales Pesados/análisis , Reciclaje , China , Medición de Riesgo
15.
Environ Pollut ; 316(Pt 2): 120654, 2023 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-36375577

RESUMEN

To understand isotope distributions of PM2.5 in residential buildings and apply them for source identification, carbon (δ13C) and lead (Pb) isotope ratios in indoor and outdoor air of residential buildings were analyzed. Moreover, factor analysis (FA) was employed to investigate sources, which were compared through isotopic analyses. The average δ13C values of indoor air are -26.94 ± 1.22‰ and -27.04 ± 0.44‰ in warm (August to October) and cold (February to March) seasons, respectively, and the corresponding values for outdoor air are -26.77 ± 0.54‰ and -26.57 ± 0.39‰. The average 206Pb/207Pb (208Pb/207Pb) ratios of indoor air are 1.1584 ± 0.0091 (2.4309 ± 0.0125) and 1.1529 ± 0.0032 (2.4227 ± 0.0081) in warm and cold seasons, respectively, and the corresponding values for outdoor air are 1.1594 ± 0.0069 (2.4374 ± 0.0103) and 1.1538 ± 0.0077 (2.4222 ± 0.0085). Seasonal variation in δ13C values or Pb isotope ratios of indoor air was not significant, and similar results were obtained for outdoor air. Significant differences were not observed between δ13C values or Pb isotope ratios of indoor and outdoor air. Traffic emission is the major contributor to indoor and outdoor PM2.5 based on isotopic analyses; this result was consistent with the results of FA. The δ13C values of indoor air in buildings with poor ventilation conditions were significantly lighter than those of outdoor air. In summary, the spatial and seasonal variations of isotopes were similar in residential buildings, which can be used to identify sources of indoor PM2.5, and ventilation condition is an influencing factor.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire Interior , Estaciones del Año , Contaminantes Atmosféricos/análisis , Contaminación del Aire Interior/análisis , Plomo , Carbono , Isótopos , Material Particulado/análisis , Monitoreo del Ambiente/métodos , Tamaño de la Partícula
16.
Chemosphere ; 313: 137368, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36574574

RESUMEN

Although antimony (Sb) contamination has been documented in urban areas, knowledge gaps remain concerning the contributions of the different sources to the Sb urban biogeochemical cycle, including non-exhaust road traffic emissions, urban materials leaching/erosion and waste incineration. Additionally, details are lacking about Sb chemical forms involved in urban soils, sediments and water bodies. Here, with the aim to document the fate of metallic contaminants emitted through non-exhaust traffic emissions in urban aquatic systems, we studied trace element contamination, with a particular focus on Sb geochemistry, in three highway stormwater pond systems, standing as models of surface environments receiving road-water runoff. In all systems, differentiated on the basis of lead isotopic signatures, Sb shows the higher enrichment factor with respect to the geochemical background, up to 130, compared to other traffic-related inorganic contaminants (Co, Cr, Ni, Cu, Zn, Cd, Pb). Measurements of Sb isotopic composition (δ123Sb) performed on solid samples, including air-exposed dusts and underwater sediments, show an average signature of 0.07 ±â€¯0.05‰ (n = 25, all sites), close to the δ123Sb value measured previously in certified reference material of road dust (BCR 723, δ123Sb = 0.03 ±â€¯0.05‰). Moreover, a fractionation of Sb isotopes is observed between solid and dissolved phases in one sample, which might result from Sb (bio)reduction and/or adsorption processes. SEM-EDXS investigations show the presence of discrete submicrometric particles concentrating Sb in all the systems, interpreted as friction residues of Sb-containing brake pads. Sb solid speciation determined by linear combination fitting of X-Ray Absorption Near Edge Structure (XANES) spectra at the Sb K-edge shows an important spatial variability in the ponds, with Sb chemical forms likely driven by local redox conditions: "dry" samples exposed to air exhibited contributions from Sb(V)-O (52% to 100%) and Sb(III)-O (<10% to 48%) species whereas only underwater samples, representative of suboxic/anoxic conditions, showed an additional contribution from Sb(III)-S (41% to 80%) species. Altogether, these results confirm the traffic emission as a specific source of Sb emission in surface environments. The spatial variations of Sb speciation observed along the road-to-pond continuum likely reflect a high geochemical reactivity, which could have important implications on Sb transfer properties in (sub)surface hydrosystems.


Asunto(s)
Antimonio , Metales Pesados , Antimonio/análisis , Estanques , Monitoreo del Ambiente/métodos , Polvo , Suelo/química , Isótopos , Metales Pesados/análisis
17.
Environ Res ; 220: 115173, 2023 03 01.
Artículo en Inglés | MEDLINE | ID: mdl-36584841

RESUMEN

Despite ongoing concerns about trace metal and metalloid (trace metals) exposure risks from indoor dust, there has been limited research examining their sources and relationship to outdoor soils. Here we determine the concentrations and sources for potentially toxic trace metals arsenic (As), chromium (Cr), copper (Cu), manganese (Mn), lead (Pb) and zinc (Zn) and their pathways into homes in Sydney, Australia, using home-matched indoor dust (n = 166), garden soil (n = 166), and road dust samples (n = 51). All trace metals were more elevated indoors versus their matched garden soil counterparts. Indoor Cu and Zn dust concentrations were significantly more enriched than outdoor dusts and soils, indicating indoor sources were more relevant for these elements. By contrast, even though Pb was elevated in indoor dust, garden soil concentrations were correspondingly high, indicating that it remains an important source and pathway for indoor contamination. Elevated concentrations of As, Pb and Zn in garden soil and indoor dust were associated with home age (>50 years), construction materials, recent renovations and deteriorating interior paint. Significant correlations (p < 0.05) between road dust and garden soil Cu concentrations, and those of As and Zn in soil and indoor dust, and Pb across all three media suggest common sources. Scanning electron microscopy (SEM) analysis of indoor dust samples (n = 6) showed that 57% of particles were derived from outdoor sources. Lead isotopic compositions of soil (n = 21) and indoor dust (n = 21) were moderately correlated, confirming the relevance of outdoor contaminants to indoor environments. This study illustrates the source, relationship and fate of trace metals between outdoor and indoor environments. The findings provide insight into understanding and responding to potentially toxic trace metal exposures in the home environment.


Asunto(s)
Metales Pesados , Contaminantes del Suelo , Oligoelementos , Exposición a Riesgos Ambientales/análisis , Metales Pesados/análisis , Ambiente en el Hogar , Plomo/análisis , Oligoelementos/análisis , Contaminantes del Suelo/análisis , Zinc/análisis , Polvo/análisis , Suelo , Monitoreo del Ambiente , Medición de Riesgo
18.
Environ Sci Pollut Res Int ; 30(2): 4269-4277, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-35971050

RESUMEN

Heavy metal contamination in urban environments, particularly lead (Pb) pollution, is a health hazard both to humans and ecological systems. Despite wide recognition of urban metal pollution in many cities, there is still relatively limited research regarding heavy metal distribution and transport at the household-scale between soils and indoor dusts-the most important scale for actual human interaction and exposure. Thus, using community-scientist-generated samples in Indianapolis, IN (USA), we applied bulk chemistry, Pb isotopes, and scanning electron microscopy (SEM) to illustrate how detailed analytical techniques can aid in interpretation of Pb pollution distribution at the household-scale. Our techniques provide definitive evidence for Pb paint sourcing in some homes, while others may be polluted with Pb from past industrial/vehicular sources. SEM revealed anthropogenic particles suggestive of Pb paint and the widespread occurrence of Fe-rich metal anthropogenic spherules across all homes, indicative of pollutant transport processes. The variability of Pb pollution at the household scale evident in just four homes is a testament to the heterogeneity and complexity of urban pollution. Future urban pollution research efforts would do well to utilize these more detailed analytical methods on community-sourced samples to gain better insight into where the Pb came from and how it currently exists in the environment. However, these methods should be applied after large-scale pollution screening techniques such as portable X-ray fluorescence (XRF), with more detailed analytical techniques focused on areas where bulk chemistry alone cannot pinpoint dominant pollution mechanisms and where community scientists can also give important metadata to support geochemical interpretations.


Asunto(s)
Contaminantes Ambientales , Metales Pesados , Contaminantes del Suelo , Humanos , Monitoreo del Ambiente/métodos , Plomo , Contaminación Ambiental , Contaminantes Ambientales/análisis , Metales Pesados/análisis , Ciudades , Suelo , Medición de Riesgo , Contaminantes del Suelo/análisis , China
19.
Environ Sci Technol ; 56(18): 13107-13118, 2022 09 20.
Artículo en Inglés | MEDLINE | ID: mdl-36083611

RESUMEN

Industrial activities release aerosols containing toxic metals into the atmosphere, where they are transported far from their sources, impacting ecosystems and human health. Concomitantly, long-range-transported mineral dust aerosols play a role in Earth's radiative balance and supply micronutrients to iron-limited ecosystems. To evaluate the sources of dust and pollutant aerosols to Alaska following the 2001 phase-out of leaded gasoline in China, we measured Pb-Sr-Nd isotopic compositions of particles collected in 2016 from snow pits across an elevational transect (2180-5240 m-a.s.l) in Denali National Park, USA. We also determined Pb flux and enrichment from 1991-2011 in the Denali ice core (3870 m-a.s.l). Chinese coal-burning and non-ferrous metal smelting account for up to 64% of Pb deposition at our sites, a value consistent across the western Arctic. Pb isotope ratios in the aerosols did not change between 2001 and 2016, despite the ban on lead additives. Emissions estimates demonstrate that industrial activities have more than compensated for the phase-out of leaded gasoline, with China emitting ∼37,000 metric tons year-1 of Pb during 2013-2015, approximately 78% of the Pb from East Asia. The Pb flux to Alaska now equals that measured in southern Greenland during peak pollution from North America.


Asunto(s)
Polvo , Contaminantes Ambientales , Aerosoles/análisis , China , Carbón Mineral , Ecosistema , Monitoreo del Ambiente , Gasolina , Humanos , Hierro , Isótopos , Plomo , Micronutrientes
20.
Environ Sci Pollut Res Int ; 29(57): 85815-85828, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36125684

RESUMEN

In this study, the anthropogenic contamination in Trasimeno lake (Central Italy) was investigated using three sediment cores spanning over the last 150 years (Anthropocene) to identify the primary sources of pollution and quantify the level of contaminant enrichment in the basin. First, based on the relative cumulative frequency and linear regression methods, we obtained a geochemical baseline for the lake using the deeper parts of the sediment cores. The geochemical baseline allowed us to determine the values of trace elements enrichment factors. On this knowledge, as a second result, we were able to reconstruct the natural sources and the anthropogenic impact on the lake with a biennial resolution. This goal has been obtained by combining different inorganic and organic chemical proxies such as trace elements, polycyclic aromatic hydrocarbons, and lead isotope ratios and exploiting both principal component and factor analysis to associate chemical proxies to human-driven contamination processes. Five different groups of elements have been identified, one of which is of natural origin and four of anthropogenic origin. In particular, it was possible to identify the times and impacts of the industrial activities during the Second World War, which dispersed heavy metals in sediments. Moreover, we found evidence of the recent human activities that have characterized the surroundings of the basin, such as Pb inputs related to the use of gasoline and the enrichment of certain elements generally used in agricultural activities (such as P, Cu, and Mn) due to the development of this sector in the last 40 years.


Asunto(s)
Metales Pesados , Hidrocarburos Policíclicos Aromáticos , Oligoelementos , Contaminantes Químicos del Agua , Humanos , Oligoelementos/análisis , Hidrocarburos Policíclicos Aromáticos/análisis , Sedimentos Geológicos/química , Monitoreo del Ambiente/métodos , Contaminantes Químicos del Agua/análisis , Lagos/química , Metales Pesados/análisis
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