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1.
Environ Sci Technol ; 58(24): 10504-10514, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38838208

RESUMO

Some persistent hydrophobic pollutants biomagnify, i.e., achieve higher contaminant levels in a predator than in its prey (Cpredator/Cprey > 1). This ratio is called the biomagnification factor (BMF) and is traditionally determined using tissues from carcasses or biopsies. Using a noninvasive method that relies on equilibrium sampling in silicone-film-coated vessels and chemical analysis of paired diet and feces, we determined on three occasions the thermodynamic biomagnification limit (BMFlim) and feces-based biomagnification factor (BMFF) for three zoo-housed polar bears who experience seasonal periods of hyperphagia and hypophagia. All bears had high biomagnification capabilities (BMFlim was up to 200) owing to very efficient lipid assimilation (up to 99.5%). The bears differed up to a factor of 3 in their BMFlim. BMFlim and BMFF of a bear increased by up to a factor of 4 during the hypophagic period, when the ingestion rate was greatly reduced. Much of that variability can be explained by differences in the lipid assimilation efficiency, even though this efficiency ranged only from 98.1 to 99.5%. A high BMFlim was associated with a high abundance of Bacteroidales and Lachnospirales in the gut microbiome. Biomagnification varies to a surprisingly large extent between individuals and within the same individual over time. Future work should investigate whether this can be attributed to the influence of the gut microbiome on lipid assimilation by studying more individual bears at different key physiological stages.


Assuntos
Microbioma Gastrointestinal , Ursidae , Animais , Fezes/microbiologia , Dieta
2.
Environ Res ; 245: 118053, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38160976

RESUMO

The middle reaches of the Yellow River are rich in energy resources, with the Kuye River, a first-class river in this region, serving as a vital hub for the coal chemical industry within China. This study investigated the occurrence patterns, environmental trends, and ecological risks associated with polycyclic aromatic hydrocarbons (PAHs) in the Kuye River Basin, offering insights into the environmental dynamics of regions. The findings indicated that the river sediments primarily contained PAHs with medium to high-molecular weights, exhibiting levels ranging from 402.92 ng/g dw to 16,783.72 ng/g dw, while water bodies predominantly featured PAHs with low to medium molecular weights, ranging from 299.34 ng/L to 10,930.9 ng/L. The source analysis of PAHs indicated that industrial and traffic exhaust emissions were the primary contributors to PAHs in the Kuye basin, with sediments serving as a secondary release source based on fugacity fraction. The content of PAHs in sediment correlated closely with the environmental factors, and the PAHs inventory of the basin was 19.97 tons. The increased overall PAH concentration in the basin posed significant ecological and public health concerns, necessitating urgent attention.


Assuntos
Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Monitoramento Ambiental , Hidrocarbonetos Policíclicos Aromáticos/análise , Sedimentos Geológicos/análise , Poluentes Químicos da Água/análise , Rios/química , China , Medição de Risco , Água
3.
Proc Natl Acad Sci U S A ; 118(45)2021 11 09.
Artigo em Inglês | MEDLINE | ID: mdl-34725159

RESUMO

Refractory oxygen bound to cations is a key component of the interior of rocky exoplanets. Its abundance controls planetary properties including metallic core fraction, core composition, and mantle and crust mineralogy. Interior oxygen abundance, quantified with the oxygen fugacity (fO2), also determines the speciation of volatile species during planetary outgassing, affecting the composition of the atmosphere. Although melting drives planetary differentiation into core, mantle, crust, and atmosphere, the effect of fO2 on rock melting has not been studied directly to date, with prior efforts focusing on fO2-induced changes in the valence ratio of transition metals (particularly iron) in minerals and magma. Here, melting experiments were performed using a synthetic iron-free basalt at oxygen levels representing reducing (log fO2 = -11.5 and -7) and oxidizing (log fO2 = -0.7) interior conditions observed in our solar system. Results show that the liquidus of iron-free basalt at a pressure of 1 atm is lowered by 105 ± 10 °C over an 11 log fO2 units increase in oxygen abundance. This effect is comparable in size to the well-known enhanced melting of rocks by the addition of H2O or CO2 This implies that refractory oxygen abundance can directly control exoplanetary differentiation dynamics by affecting the conditions under which magmatism occurs, even in the absence of iron or volatiles. Exoplanets with a high refractory oxygen abundance exhibit more extensive and longer duration magmatic activity, leading to more efficient and more massive volcanic outgassing of more oxidized gas species than comparable exoplanets with a lower rock fO2.

4.
Proc Natl Acad Sci U S A ; 118(40)2021 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-34588307

RESUMO

Bridgmanite, the most abundant mineral of the Earth's lower mantle, has been reported in only a few shocked chondritic meteorites; however, the compositions of these instances differ from that expected in the terrestrial bridgmanite. Here, we report the first natural occurrence of Fe-bearing aluminous bridgmanite in shock-induced melt veins within the Katol L6 chondrite with a composition that closely matches those synthesized in high-pressure and temperature experiments over the last three decades. The Katol bridgmanite coexists with majorite and metal-sulfide intergrowths. We found that the natural Fe-bearing aluminous bridgmanite in the Katol L6 chondrite has a significantly higher Fe3+/ΣFe ratio (0.69 ± 0.08) than coexisting majorite (0.37 ± 0.10), which agrees with experimental studies. The Katol bridgmanite is arguably the closest natural analog for the bridgmanite composition expected to be present in the Earth's lower mantle. Textural observations and comparison with laboratory experiments suggest that the Katol bridgmanite formed at pressures of ∼23 to 25 gigapascals directly from the chondritic melt generated by the shock event. Thus, the Katol L6 sample may also serve as a unique analog for crystallization of bridgmanite during the final stages of magma ocean crystallization during Earth's formation.

5.
Environ Res ; 238(Pt 2): 117225, 2023 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-37788759

RESUMO

Antibiotics have been heavily used over the past decades, resulting in their frequent detections in rivers and increasing ecological risks. Recognizing characteristics of antibiotic ecological risks (AERs) and making effective strategies to mitigate the AERs are essential to ensure the safety of aquatic ecosystem and public health. In this study, an integrated technological framework has been proposed toward identifying management options for reducing AERs by jointly utilizing multimedia fugacity modelling and ecotoxicological risk assessment, and applied to characterize the AERs in a peri-urban river in Beijing. Specifically, a level III fugacity model has been successfully established to simulate the fate of antibiotics in the environment, and the manageable parameters have been screened out via sensitivity analysis of the model. Then the validated fugacity model has been used for scenario modellings to optimize mitigation strategies of AERs. Results show most of the antibiotics considered are frequently detected in the river, and pose medium or high risks to aquatic organisms. Relatively, the macrolides and fluoroquinolones present higher ecotoxicological risks than sulfonamides and tetracyclines. Furthermore, the mixture risk quotient and predictive equation of concentration addition suggest joint and synergistic/antagonistic effects of AERs for multiple or binary antibiotics in the environment. Largely, the concentrations of antibiotics in the river are determined by the source emissions into water and soil. Scenario modellings show the improvement of antibiotic removal rates would be considered preferentially to mitigate the AERs. Also, controlling human consumption is conducive to reducing the risks posed by tetracyclines, macrolides and trimethoprim, while controlling animal consumption would benefit the reduction for sulfonamides. Overall, the joint strategy presents the greatest reduction of AERs by reducing antibiotic consumption and together improving sewage treatment rate and antibiotic removal rate. The study provides us a useful guideline to make ecological risk-based mitigation strategy for reducing AERs in environment.


Assuntos
Antibacterianos , Poluentes Químicos da Água , Animais , Humanos , Antibacterianos/análise , Rios , Multimídia , Ecossistema , Sulfanilamida , Macrolídeos/análise , Tetraciclinas/análise , China , Monitoramento Ambiental/métodos , Poluentes Químicos da Água/análise , Medição de Risco
6.
Environ Res ; 238(Pt 2): 117238, 2023 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-37783324

RESUMO

The potential human health risks associated with soil vapor intrusion and volatile organic compounds (VOCs) exposure were characterized at an industrialized site by the quantification of gaseous VOCs in soil pores using a passive sampling technique. The gaseous tetrachloroethene (PCE) in soil pores varied between 12 and 5,400 µg m-3 showing 3 orders of magnitude variation with dependence on groundwater PCE concentrations. Though the PCE concentration in the air only varied between 0.45 and 1.5 µg m-3 showing negligible variations compared to the variation observed in soil pores. The PCE concentration in the air varied between 0.45 and 1.5 µg m-3. The calculation of fugacity suggested that the PCE in the test site originated from groundwater. Measured PCE in groundwater ranged from 14 to 2,400 times higher than PCE in soil gas. This indicates that conducting a vapor intrusion risk assessment using passive soil gas sampling is critical for accurate risk characterization and assessment. Estimated PCE inhalation cancer risks for street cleaners and indoor residents varied between 10-6 and 10-4 with a low plausible hazard, and between 10-3 and 10-2 with a high risk, respectively. The results of this study demonstrate that passive sampling offers a significantly lower cost and labor-intensive approach compared to traditional methods for assessing pollution distribution in contaminated sites and characterizing risks. This highlights the potential for wider application of passive sampling techniques in environmental studies.


Assuntos
Poluição do Ar em Ambientes Fechados , Água Subterrânea , Poluentes do Solo , Tetracloroetileno , Compostos Orgânicos Voláteis , Humanos , Poluição do Ar em Ambientes Fechados/análise , Solo , Monitoramento Ambiental/métodos , Poluentes do Solo/análise , Gases , Compostos Orgânicos Voláteis/análise
7.
Ecotoxicol Environ Saf ; 266: 115541, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37806132

RESUMO

Precipitation can lead to significant leaching of heavy metals from abandoned tailings,resulting in a decline in the quality of the surrounding environment. This study aimed to simulate and quantify the migration patterns and fate of heavy metals in tailings caused by precipitation in various environmental media (tailings, air, water, soil, and sediments) using leaching tests, source apportionment, and a fugacity model. Results revealed that the average contents of Cd, Cu, As, Pb, Zn, and Cr in the un-weathered tailings were 3.43, 495.56, 160.70, 138.94, 536.57, and 69.52 mg/kg, respectively. The ecological risk factors in the tailings as well as in sediments and soils, were in the following order: Cd >Cu >As >Pb >Zn >Cr. A fugacity model based on the mass-balance methods was established, achieving a good agreement between simulation and measured values. The total amounts of Cd, Cu, As, Pb, and Zn leached from abandoned tailings over the 30-year evaluation period were estimated to be 1.09, 62.44, 0.16, 0.94, and 102.12 t, respectively. Soil and sediments are important reservoirs for heavy metals. The sum of the As, Cd, Cu, Pb, and Zn storage capacities in the soil and sediment accounted for 77.28%, 75.63%, 73.94%, 69.39%, and 57.80% of the total storage capacity, respectively. This study could provide the means for the establishment of a targeted pollution control plan, a guide for restoration projects, and will aid in controlling pollution risk and improving the surrounding environment.


Assuntos
Metais Pesados , Poluentes do Solo , Monitoramento Ambiental , Cádmio , Chumbo , Medição de Risco , Poluentes do Solo/análise , Metais Pesados/análise , Solo , China
8.
Ecotoxicol Environ Saf ; 263: 115286, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37481858

RESUMO

The comprehensive understanding of PCBs' fate has been impeded by the lack of simultaneous monitoring of PCBs in multiple environmental media in the background areas, which were considered long-term sinks for highly chlorinated PCBs. To address this gap, this study analyzed soils, willow tree barks, water, suspended particulate matter (SPM), and sediment samples collected from the middle reach of the Huaihe River in China for 27 PCBs. The results showed that the levels of ∑27PCBs in the soils were comparable to or lower than the background values worldwide. There were no significant correlations between organic matter and ∑27PCB concentrations in the soils and sediments. Additionally, the contamination of dioxin-like PCBs in the aquatic environment of the study area deserves more attention than in the soils. Applying the level III fugacity model to PCB 52, 77, 101, and 114 revealed that the soil was the primary reservoir, and air-soil exchange was the dominant intermedia transfer process, followed by air-water exchange. Furthermore, simulated results of air-soil and air-water diffusion were compared with those calculated from the field concentrations to predict the potential environmental behaviors of PCBs. Results indicated that the studied river would be a "secondary source" for PCB 52, 77, and 101. However, PCB 52, 77, 101, and 114 would continue to transfer from the air to the soil. This study combines multimedia field measurements and the fugacity model, providing a novel approach to predicting the potential environmental behaviors of PCBs.


Assuntos
Bifenilos Policlorados , Bifenilos Policlorados/análise , Multimídia , Monitoramento Ambiental/métodos , Água , Solo
9.
Environ Geochem Health ; 45(10): 7405-7424, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-36788152

RESUMO

This study investigated the sources, contamination and ecological risks of polycyclic aromatic hydrocarbons (PAHs) based on their spatiotemporal distribution in aquatic environment in the Wuhan section of the Yangtze River (WYR). The fugacity ratio evaluation indicated that sediment was secondary release sources of two- and three-ring PAHs and sinks of four- and five-ring PAHs. The total concentrations of PAHs (Σ16PAHs) ranged from 2.51 to 102.5 ng/L in water with the dominant contribution of 47.8% by two-ring PAHs. Σ16PAHs in sediments varied from 5.90 to 2926 ng/g with the contribution of 35.4% by four-ring PAHs. The higher levels of PAHs occurred around developed industrial areas during the wet season, which was related to local industrial emissions and influenced by rainfall/runoff. Annual flux of Σ16PAHs was estimated of 28.77 t. The PMF model analysis revealed that petroleum and industrial emissions were the dominant sources in water accounting for 58.5% of the total pollution, although traffic emission was the main source for sediment accounting for 44.6%. Risk assessments showed that PAHs in water were at low risks, whereas about 44% of the sediments were identified as medium risks. Therefore, energy structure adjustment and further implement of regulation and monitoring are necessary to reduce PAH emissions.


Assuntos
Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Hidrocarbonetos Policíclicos Aromáticos/análise , Rios/química , Monitoramento Ambiental , Poluentes Químicos da Água/análise , Sedimentos Geológicos/química , China
10.
Environ Sci Technol ; 56(13): 9497-9504, 2022 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-35593505

RESUMO

In a proof-of-concept study, we recently used equilibrium sampling with silicone films to noninvasively derive the thermodynamic limit to a canine's gastrointestinal biomagnification capability (BMFlim) by determining the ratio of the products of the volume (V) and fugacity capacity (Z) of food and feces. In that earlier study, low contaminant levels prevented the determination of contaminant fugacities (f) in food and feces. For zoo-housed polar bears, fed on a lipid-rich diet of fish and seal oil, we were now able to measure the increase in f of nine native polychlorinated biphenyls (PCBs) upon digestion, providing incontestable proof of the process of gastrointestinal biomagnification. A high average BMFlim value of ∼171 for the bears was caused mostly by a remarkable reduction in fugacity capacity driven by a high lipid assimilation capacity. Lipid-rich diets increase the uptake of biomagnifying contaminants in two ways: because they tend to have higher contaminant concentrations and because they lead to a high Z value drop during digestion. We also confirmed that equilibrium sampling yielded similar Z values for PCBs originally present in food and feces and for isotopically labeled PCBs spiked onto those samples, which makes the method suitable for investigating the biomagnification capability of organisms, even if native contaminant concentrations in their diet and feces are low.


Assuntos
Bifenilos Policlorados , Ursidae , Animais , Bioacumulação , Dieta , Cães , Fezes , Lipídeos , Termodinâmica
11.
Environ Sci Technol ; 56(7): 4017-4028, 2022 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-35311252

RESUMO

We now know that nanoplastics can harm aquatic organisms, but understanding ecological risk starts with understanding fate. We coupled population balance and fugacity models to predict the conditions under which nanoplastics remain as single particles, aggregate, or sediment and to predict their capacity to concentrate organic pollutants. We carried out simulations across a broad range of nanoplastic concentrations, particle sizes, and particle-particle interactions under a range of salinity and organic matter conditions. The model predicts that across plastic materials and environmental conditions, nanoplastics will either remain mostly dispersed or settle as aggregates with natural colloids. Nanoplastics of different size classes respond dissimilarly to concentration, ionic strength, and organic matter content, indicating that the sizes of nanoplastics to which organisms are exposed likely shift across ecological zones. We implemented a fugacity model of the Great Lakes to assess the organic pollution payload carried by nanoplastics, generating the expectation that nanoplastics would carry nine times more pollutants than microsized plastics and a threshold concentration of 10 µg/L at which they impact pollutant distribution. Our simulations across a broad range of factors inform future experimentation by highlighting the relative importance of size, concentration, material properties, and interactions in driving nanoplastic fate in aquatic environments.


Assuntos
Microplásticos , Poluentes Químicos da Água , Organismos Aquáticos , Tamanho da Partícula , Plásticos , Salinidade , Poluentes Químicos da Água/análise
12.
Environ Sci Technol ; 56(18): 13058-13065, 2022 09 20.
Artigo em Inglês | MEDLINE | ID: mdl-36067451

RESUMO

Leaf-air partition coefficient (Kleaf-air) values are needed to understand and predict pesticide volatilization and persistence in agroecosystems. The objectives of this work were to measure Kleaf-air values and foliar penetration for the insecticide chlorpyrifos (as an active ingredient alone and in a pesticide formulation) on alfalfa (lucerne) leaves at a range of temperatures and relative humidities and when using leaves collected in different summer months. Kleaf-air values were measured using a solid-phase fugacity meter. A portion of the leaves were also used for foliar penetration experiments. Kleaf-air values for chlorpyrifos as an active ingredient alone decreased with temperature, while the effects of temperature on chlorpyrifos in the formulation were negligible. No correlations between Kleaf-air values and relative humidity were observed. Foliar penetration increased with temperature for chlorpyrifos both as an active ingredient and in the formulation. Increasing foliar penetration with temperature is attributed to increasing diffusion into inner leaf layers. Both volatilization and foliar penetration affect the measured Kleaf-air values, so understanding the link between these processes is necessary to predict Kleaf-air values. The leaf collection date had a substantial effect on the measured Kleaf-air values, highlighting the need for a better understanding of the role of leaf properties on Kleaf-air.


Assuntos
Clorpirifos , Inseticidas , Praguicidas , Umidade , Inseticidas/análise , Praguicidas/análise , Folhas de Planta/química , Temperatura
13.
Proc Natl Acad Sci U S A ; 116(18): 8746-8755, 2019 04 30.
Artigo em Inglês | MEDLINE | ID: mdl-30975756

RESUMO

A rise in atmospheric O2 levels between 800 and 400 Ma is thought to have oxygenated the deep oceans, ushered in modern biogeochemical cycles, and led to the diversification of animals. Over the same time interval, marine sulfate concentrations are also thought to have increased to near-modern levels. We present compiled data that indicate Phanerozoic island arc igneous rocks are more oxidized (Fe3+/ΣFe ratios are elevated by 0.12) vs. Precambrian equivalents. We propose this elevation is due to increases in deep-ocean O2 and marine sulfate concentrations between 800 and 400 Ma, which oxidized oceanic crust on the seafloor. Once subducted, this material oxidized the subarc mantle, increasing the redox state of island arc parental melts, and thus igneous island arc rocks. We test this using independently compiled V/Sc ratios, which are also an igneous oxybarometer. Average V/Sc ratios of Phanerozoic island arc rocks are elevated (by +1.1) compared with Precambrian equivalents, consistent with our proposal for an increase in the redox state of the subarc mantle between 800 and 400 Ma based on Fe3+/ΣFe ratios. This work provides evidence that the more oxidized nature of island arc vs. midocean-ridge basalts is related to the subduction of material oxidized at the Earth's surface to the subarc mantle. It also indicates that the rise of atmospheric O2 and marine sulfate to near-modern levels by the late Paleozoic influenced not only surface biogeochemical cycles and animal diversification but also influenced the redox state of island arc rocks, which are building blocks of continental crust.

14.
J Environ Manage ; 319: 115652, 2022 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-35820309

RESUMO

In this study, a universal method that combined fixed-point monitoring and numerical simulation was used to understand the source, fate and risks of antibiotics in environment. Results showed that the antibiotic concentration in vegetables, soil and manure from 53 fixed-point monitoring sampling sites were ND-18.47, ND-1438.50 and ND-24710.00 µg kg-1, respectively. There were positive correlations between the antibiotic concentrations of vegetables and soil as well as between soil and manure. The average Amountsoil/manure values were 1.48-46.02, indicating that antibiotics built up pseudo persistent residues in soil due to repeated fertilization. The modified level-III fugacity model showed that tetracyclines and fluoroquinolones tend to remain in soil given their sorption and mobility, while sulfonamides were highly distributed in plants, especially in leaves. Norfloxacin, ofloxacin, sulfadiazine, sulfamethoxazole and sulfisoxazole were found to be risk factors in facility agriculture and should be continuously monitored during agricultural production. Most importantly, we used the inversion method to determine the recommended maximum residue limits of antibiotics in soil. This will not only allow for better control of the amount of the antibiotics in the environment, but also act as a potential method to assess the risks of pollutants without maximum residue limits in the environment.


Assuntos
Poluentes do Solo , Solo , Agricultura , Antibacterianos/análise , Monitoramento Ambiental/métodos , Esterco/análise , Solo/química , Poluentes do Solo/análise , Verduras
15.
J Environ Manage ; 319: 115758, 2022 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-35982562

RESUMO

Pesticide pollution has been one serious ecological and environmental issue due to its wide application, high toxicity, and complex environmental behavior. The fugacity model has been widely used to quantify biogeochemical cycles of pesticides due to its clear compartments, simple structure, and easy-accessible data. However, the lack of detailed hydrological processes limits its application for large and heterogeneous watershed. In present study, a new framework was proposed through integration of hydrological processes of SWAT and pesticide fate of fugacity model, and was applied into a typical watershed in the Three Gorges Reservoir Area, China. The results showed that surface runoff, soil erosion, and percolation varied spatiotemporally, which highlighted the importance of considering regional and seasonal heterogeneity of pesticide transport variables in the fugacity model. The amount of dichlorvos (DDV) and chlorpyrifos (CHP) in air, water, soil, and sediment phase were estimated as 0.26 kg, 19.77 kg, 1.06 × 104 kg, and 0.55 kg, respectively. Spatiotemporally, pesticide concentrations in water phase peaked in summer, while the middle and southwest regions of the watershed were identified as the hotspots for pesticide pollution. Compared with the classical model, the new framework provided technical support for the pesticide assessment at watershed scale with heterogeneous hydrological conditions, which can be easily extended to other watersheds, and integrated with other models for comprehensive agricultural management.


Assuntos
Praguicidas , Poluentes Químicos da Água , Monitoramento Ambiental/métodos , Modelos Teóricos , Multimídia , Praguicidas/análise , Água , Poluentes Químicos da Água/análise
16.
J Environ Manage ; 302(Pt B): 114096, 2022 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-34775339

RESUMO

To quantitate the degradation rate of 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta-[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronaphthalene (AHTN) under field conditions, a level III fugacity model combined with a least-squares method was used to determine the degradation rate of HHCB and AHTN in the North Canal River watershed of Beijing, China. Model fitting, validation, sensitivity, and uncertainty analyses revealed that the established model was stable and robust. The degradation rates of HHCB and AHTN were 4.16 × 10-3 h-1 (t1/2 = 167 h) and 1.68 × 10-2 h-1 (t1/2 = 41.3 h), respectively. The calculated degradation rates were extrapolated to the Liangshui River, and indicated that the differences between the measured and predicted concentrations were less than 0.32 and 0.34 log units for HHCB and AHTN, respectively. The attenuation rates of HHCB and AHTN were calculated, and the results indicated that degradation was an important yet not the sole contributor to the degradation of the polycyclic musks. Results of uncertainty analyses indicated that the inflow and outflow concentrations of the polycyclic musks in the surface water of each segment strongly influenced the model outputs, followed by environmental factors (water depth and flow rate). It is essential to measure the degradation rate in the field because of the influence of the surrounding environment. The present study reveals the utility of fugacity models to quantify the degradation rate of organic micropollutants in the field.


Assuntos
Rios , Poluentes Químicos da Água , Pequim , Benzopiranos/análise , Monitoramento Ambiental , Tetra-Hidronaftalenos/análise , Poluentes Químicos da Água/análise
17.
J Environ Manage ; 305: 114436, 2022 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-34999447

RESUMO

The impact of sluice operations on the distribution and fate of perfluoroalkyl acids (PFAAs) remains poorly understood. In this study, the distribution of PFAAs was investigated in water, suspended particles, sediment, and pore water from the upstream and downstream sections of six sluice gates along the Wangyu River, China. The target PFAAs were widely distributed in the dissolved phase (∑PFAAs: 447.61 ± 180.26 ng/L), particle phase (∑PFAAs: 2040.95 ± 1870.88 ng/g dw), sedimentary phase (∑PFAAs: 39.42 ± 35.38 ng/g dw), and pore water phase (∑PFAAs: 8172.54 ± 4278.60 ng/L). Our data suggest predominant detections of short-chain PFAAs such as perfluorobutanoic acid (PFBA) and perfluorohexanoic acid (PFHxA) in the four environmental media. Sediment pore water appeared as an essential repository and potential source for PFAA re-release to the river environment. The levels of PFAAs in the dissolved and suspended particle phase upstream of the sluices were significantly lower than those downstream, while the situation in the sediment and pore water phase was the opposite. Sluice operation caused PFAA redistribution among the multi-environment media but did not change the PFAA composition, which had the significant effect on the partition behavior of perfluoroalkyl carboxylic acids (PFCAs) between particles and water, as well as changed the migration pattern of PFOA, PFNA and PFOS from equilibrium to the migration state. Quantitative prediction models were developed for simulating fate of PFAAs in gate-controlled river, and the major factors affecting the distribution and fate of PFAAs were identified. Our findings provide insights into the redistribution mechanisms of PFAAs and an understanding of their environmental fate.


Assuntos
Ácidos Alcanossulfônicos , Fluorocarbonos , Poluentes Químicos da Água , China , Monitoramento Ambiental , Fluorocarbonos/análise , Rios , Poluentes Químicos da Água/análise
18.
Environ Sci Technol ; 55(20): 13932-13941, 2021 10 19.
Artigo em Inglês | MEDLINE | ID: mdl-34590828

RESUMO

Trophic magnification of cyclic volatile methyl siloxanes (cVMS) in a terrestrial food web was investigated by measuring concentrations of octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) and two reference chemicals within air and biota samples from an avian food web located in a mixed urban-agricultural landscape. Terrestrial trophic magnification factors derived from lipid normalized concentrations (TMFLs) for D5 and D6 were 0.94 (0.17 SE) and 1.1 (0.23 SE) and not statistically different from 1 (p > 0.05); however, the TMFL of D4 was 0.62 (0.11 SE) and statistically less than 1 (p < 0.001). TMFLs of PCB-153 and p,p'-DDE were 5.6 (2.2 SE) and 6.1 (2.8 SE) and statistically greater than 1 (p < 0.001). TMFLs of cVMS in this terrestrial system were similar to those reported in aquatic systems. However, trophic magnification factors derived on a fugacity basis (TMFFs), which recognize differences in body temperature and lipid composition between organisms, were greater than corresponding TMFLs primarily because a temperature-induced thermodynamic biomagnification of hydrophobic chemicals occurs when endothermic organisms consume poikilothermic organisms. Therefore, we recommend that biomagnification studies of food webs including endothermic and poikilothermic organisms incorporate differences in body temperature and tissue composition to accurately characterize the biomagnification potential of chemicals.


Assuntos
Cadeia Alimentar , Poluentes Químicos da Água , Bioacumulação , Temperatura Corporal , Monitoramento Ambiental , Siloxanas/análise , Temperatura , Poluentes Químicos da Água/análise
19.
Environ Sci Technol ; 55(14): 10012-10024, 2021 07 20.
Artigo em Inglês | MEDLINE | ID: mdl-34218659

RESUMO

We aimed to identify patterns in the internal distribution of persistent organic pollutants (POPs) and assess contributing factors using sea turtles and their offspring as a case study of a long-lived wildlife species. We systematically synthesized 40 years of data and developed a lipid database to test whether lipid-normalized POP concentrations are equal among tissues as expected under steady state for lipophilic compounds. Results supported equal partitioning among tissues with high blood flow or perfusion including the heart, kidney, muscle, and lung. Observed differences in the brain, fat, and blood plasma, however, suggest the physiological influence of the blood-brain barrier, limited perfusion, and protein content, respectively. Polybrominated diphenyl ethers partitioned comparably to legacy POPs. Polycyclic aromatic hydrocarbons, meanwhile, partitioned more into the lung, colon, and muscle compared to the liver under chronic and acute field exposure. Partitioning ratios of individual POPs among tissues were significantly related to the lipophilicity of compounds (as estimated by Kow) in half of the observed cases, and significant differences between juveniles and adults underscore physiological differences across life stages. The comprehensive tissue partitioning patterns presented here provide a quantitative basis to support comparative assessments of POP pollution derived from biomonitoring among multiple tissues.


Assuntos
Poluentes Ambientais , Bifenilos Policlorados , Tartarugas , Poluentes Químicos da Água , Animais , Monitoramento Ambiental , Poluentes Ambientais/análise , Éteres Difenil Halogenados/análise , Poluentes Orgânicos Persistentes
20.
Entropy (Basel) ; 23(2)2021 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-33567624

RESUMO

The micro-canonical, canonical, and grand canonical ensembles of walks defined in finite connected undirected graphs are considered in the thermodynamic limit of infinite walk length. As infinitely long paths are extremely sensitive to structural irregularities and defects, their properties are used to describe the degree of structural imbalance, anisotropy, and navigability in finite graphs. For the first time, we introduce entropic force and pressure describing the effect of graph defects on mobility patterns associated with the very long walks in finite graphs; navigation in graphs and navigability to the nodes by the different types of ergodic walks; as well as node's fugacity in the course of prospective network expansion or shrinking.

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