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Per- and polyfluoroalkyl substance (PFAS) retention by colloidal activated carbon (CAC) using dynamic column experiments Полный текст
2022
Niarchos, Georgios | Ahrens, Lutz | Kleja, Dan Berggren | Fagerlund, Fritjof
Per- and polyfluoroalkyl substance (PFAS) retention by colloidal activated carbon (CAC) using dynamic column experiments Полный текст
2022
Niarchos, Georgios | Ahrens, Lutz | Kleja, Dan Berggren | Fagerlund, Fritjof
Developing effective remediation methods for per- and polyfluoroalkyl substance (PFAS)-contaminated soils is a substantial step towards counteracting their widespread occurrence and protecting our ecosystems and drinking water sources. Stabilisation of PFAS in the subsurface using colloidal activated carbon (CAC) is an innovative, yet promising technique, requiring better understanding. In this study, dynamic soil column tests were used to assess the retardation of 10 classical perfluoroalkyl acids (PFAAs) (C₅–C₁₁ perfluoroalkyl carboxylic acids (PFCAs) and C₄, C₆, C₈ perfluoroalkane sulfonates (PFSAs)) as well as two alternative PFAS (6:2 and 8:2 fluorotelomer sulfonates) using CAC at 0.03% w/w, to investigate the fate and transport of PFAS under CAC treatment applications. Results showed high retardation rates for long-chain PFAS and eight times higher retardation for the CAC-treated soil compared to the non-treated reference soil for the ∑PFAS. Replacement of shorter chain perfluorocarboxylic acids (PFCAs), such as perfluoropentanoic acid (PFPeA), by longer chained PFAS was observed, indicating competition effects. Partitioning coefficients (Kd values) were calculated for the CAC fraction at ∼10³–10⁵ L kg⁻¹ for individual PFAS, while there was a significant positive correlation (p < 0.05) between perfluorocarbon chain length and Kd. Mass balance calculations showed 37% retention of ∑PFAS in treated soil columns after completion of the experiments and 99.7% higher retention rates than the reference soil. Redistribution and elution of CAC were noticed and quantified through organic carbon analysis, which showed a 23% loss of carbon during the experiments. These findings are a step towards better understanding the extent of CAC's potential for remediation of PFAS-contaminated soil and groundwater and the limitations of its applications.
Показать больше [+] Меньше [-]Per- and polyfluoroalkyl substance (PFAS) retention by colloidal activated carbon (CAC) using dynamic column experiments Полный текст
2022
Niarchos, Georgios | Ahrens, Lutz | Berggren Kleja, Dan | Fagerlund, Fritjof
Developing effective remediation methods for per- and polyfluoroalkyl substance (PFAS)-contaminated soils is a substantial step towards counteracting their widespread occurrence and protecting our ecosystems and drinking water sources. Stabilisation of PFAS in the subsurface using colloidal activated carbon (CAC) is an innovative, yet promising technique, requiring better understanding. In this study, dynamic soil column tests were used to assess the retardation of 10 classical perfluoroalkyl acids (PFAAs) (C-5-C-11 perfluoroalkyl carboxylic acids (PFCAs) and C-4, C-6, C-8 perfluoroalkane sulfonates (PFSAs)) as well as two alternative PFAS (6:2 and 8:2 fluorotelomer sulfonates) using CAC at 0.03% w/w, to investigate the fate and transport of PFAS under CAC treatment applications. Results showed high retardation rates for long-chain PFAS and eight times higher retardation for the CAC-treated soil compared to the non-treated reference soil for the Sigma PFAS. Replacement of shorter chain perfluorocarboxylic acids (PFCAs), such as perfluoropentanoic acid (PFPeA), by longer chained PFAS was observed, indicating competition effects. Partitioning coefficients (K-d values) were calculated for the CAC fraction at similar to 10(3)-10(5) L kg(-1) for individual PFAS, while there was a significant positive correlation (p < 0.05) between perfluorocarbon chain length and K-d. Mass balance calculations showed 37% retention of Sigma PFAS in treated soil columns after completion of the experiments and 99.7% higher retention rates than the reference soil. Redistribution and elution of CAC were noticed and quantified through organic carbon analysis, which showed a 23% loss of carbon during the experiments. These findings are a step towards better understanding the extent of CAC's potential for remediation of PFAS-contaminated soil and groundwater and the limitations of its applications.
Показать больше [+] Меньше [-]Accumulation and depuration of microplastic fibers, fragments, and tire particles in the eastern oyster, Crassostrea virginica: A toxicokinetic approach Полный текст
2022
Weinstein, John E. | Ertel, Bonnie M. | Gray, Austin D.
Along the South Carolina coast (U.S.) where the ecologically and economically important eastern oyster (Crassostrea virginica) forms extensive intertidal reefs, recent surface water surveys found that fibers, fragments, and microscopic tire particles represented 43.6%, 30.9%, and 17.7% of the total microplastics, respectively. The aim of this study was to characterize accumulation and depuration of these particles in eastern oysters. Oysters were exposed to purple polyethylene fibers, green nylon fragments, or micronized crumb rubber at a concentration of 5000 microplastics/L, and sacrificed after 0, 24, 48, and 96 h to characterize uptake. Following 96 h, remaining oysters were transferred to microplastic-free brackish water and sacrificed at 24, 48, and 96 h to characterize depuration. For fibers and fragments, levels increased in a nonlinear fashion reaching 1.61 ± 0.6 particles/g w. w. (mean ± SE) and 0.46 ± 0.1 particles/g w. w. after 96 h, respectively. Conditional uptake clearance rate constants (kᵤ) were estimated to be 0.0084 and 0.0025 mL/g*h for fibers and fragments, respectively. For crumb rubber, levels increased in a linear fashion reaching 3.62 ± 0.8 particles/g w. w. after 96 h, and the kᵤ value was estimated to be 0.0077 mL/g*h. Depuration was best described using a two-compartment (double exponential) model suggesting the presence of fast and slow compartments. Conditional depuration rate constants (kd) for the slow compartments were 0.0084, 0.0205, and 0.0048/h for fibers, fragments, and crumb rubber, respectively. These results demonstrate accumulation and depuration of microplastics in eastern oysters is size-and shape-dependent. Depuration, which is a common practice for shellfish safety, is an effective way to reduce microplastic loads in eastern oysters, but the minimum recommended time of 44 h would only reduce loads of these particles by 55.5–67.6%.
Показать больше [+] Меньше [-]Organic contaminants in imported salmon feed and their effects on reef ecosystems in New Zealand Полный текст
2022
McMullin, Rebecca M. | Chen, Ruiwen | Niu, Shan | Matthews, Will | Murschell, Trey | Wing, Stephen R. | Hageman, Kimberly J.
Organic matter from salmon farms has been shown to be assimilated by soft sediment and rocky reef communities within the ecological footprint of salmon farms. Given these findings, another question arises – What other chemicals in salmon feed may be assimilated into wild communities via organic waste from salmon farms? Here we measured a suite of organic contaminants in salmon feed, in organisms used in a controlled feeding experiment, and in reef species collected within the depositional footprint of salmon farms. Gas Chromatography-Tandem Mass Spectrometry was used to quantify trace concentrations of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and current-use (CPUs) and historic-use pesticides (HUPs) in salmon feed imported to New Zealand. The effect of assimilation of farm-derived organic matter on contaminant profiles differed among species during the controlled feeding experiment and demonstrated that migration of individuals to a farm-associated site has the potential to increase or decrease organic contaminant concentrations. Concentrations of PCBs in Parapercis colias (blue cod), a highly resident, long-lived fish, were significantly higher at farm sites than at reference sites. While these concentrations were relatively low in a global context, this result presents blue cod as an important candidate for future monitoring of organic contaminants around point sources. PCBs and PBDEs measured in wild marine species were all below limits set by the European Union, whereas concentrations of certain HUPs, specifically dichlorodiphenyltrichloroethane (DDT) and its degradation products and endosulfan, may be of concern as a consequence of alternative anthropogenic activities. Overall, feed imported to New Zealand had relatively low levels of most organic contaminants that, at current levels, are unlikely to result in significant ecological effects to wild communities in adjacent habitats.
Показать больше [+] Меньше [-]Effect of freeze-thaw cycle aging and high-temperature oxidation aging on the sorption of atrazine by microplastics Полный текст
2022
Sun, Shu | Sui, He | Xu, Liang | Zhang, Jiao | Wang, Dongying | Zhou, Zhenfeng
This study aims to better understand the aging characteristics of microplastics in the environment and the influence of aging microplastics on the migration and transformation of organic pollutants. In this study, polyvinyl chloride (PVC) and polyethylene (PE) were chosen as research objects, and the effects of two aging methods (freeze-thaw cycle aging and high-temperature oxidation aging) on their surface properties and atrazine (ATZ) sorption were investigated. The crystallinity of PE increased after freeze-thaw cycling and decreased after high-temperature oxidation. The freeze-thaw cycle destroys the amorphous region of PE, reducing the micropores on the PE surface and decreasing the ATZ adsorbed by PE. Although aging had no significant effect on the surface structure of PVC, it caused new oxygen-containing functional groups to be produced on the PVC surface, which reduced the ATZ adsorption capacity. These results show that the two aging modes change the surface properties of PVC and PE, thus affecting the sorption mechanism of ATZ, and provide a theoretical premise for the natural behavior and ecological chance assessment of ATZ in the presence of microplastics.
Показать больше [+] Меньше [-]Thallium distribution in an estuary affected by acid mine drainage (AMD): The Ría de Huelva estuary (SW Spain) Полный текст
2022
Cánovas, Carlos Ruiz | Basallote, María Dolores | Macías, Francisco | Freydier, Rémi | Parviainen, Annika | Pérez López, Rafael
Thallium distribution in an estuary affected by acid mine drainage (AMD): The Ría de Huelva estuary (SW Spain) Полный текст
2022
Cánovas, Carlos Ruiz | Basallote, María Dolores | Macías, Francisco | Freydier, Rémi | Parviainen, Annika | Pérez López, Rafael
This study investigates the behavior of Tl in the Ría de Huelva (SW Spain), one of the most metal polluted estuaries in the world. Dissolved Tl concentration displayed a general decrease across the estuary during the dry season (DS); from 5.0 to 0.34 μg/L in the Tinto and Odiel estuaries, respectively, to 0.02 μg/L in the channel where the rivers join. A slighter decrease was observed during the wet season (WS) (from 0.72 to 0.14 μg/L to 0.02 μg/L) due to the dilution effect of rainfalls in the watersheds. These values are 3 orders of magnitude higher than those reported in other estuaries worldwide. Different increases in Tl concentrations with salinity were observed in the upper reaches of the Tinto and Odiel estuaries, attributed to desorption processes from particulate matter. Chemical and mineralogical evidences of particulate matter, point at Fe minerals (i.e., jarosite) as main drivers of Tl particulate transport in the estuary. Unlike other estuaries worldwide, where a fast sorption process onto particulate matter commonly takes place, Tl is mainly desorbed from particulate matter in the Tinto and Odiel estuaries. Thus, Tl may be released back from jarositic particulate matter across the salinity gradient due to the increasing proportion of unreactive TlCl⁰ and K⁺ ions, which compete for adsorption sites with Tl⁺ at increasing salinities. A mixing model based on conservative elements revealed a 6-fold increase in Tl concentrations related to desorption processes. However, mining spills like that occurred in May 2017 may contribute to enhance dissolved and particulate Tl concentrations in the estuary as well as to magnify these desorption processes (up to around 1100% of Tl release), highlighting the impact of the mine spill on the remobilization of Tl from the suspended matter to the water column.
Показать больше [+] Меньше [-]Thallium distribution in an estuary affected by acid mine drainage (AMD): The Ría de Huelva estuary (SW Spain) Полный текст
2022
Ruiz Cánovas, Carlos | Basallote, María Dolores | Macías, Francisco | Freydier, Rémi | Parviainen, Annika Jenni Johana | Pérez López, Rafael
Supplementary data to this article can be found online at https://doi. org/10.1016/j.envpol.2022.119448. | This work was supported by the Spanish Ministry of Economy and Competitiveness under the research projects CAPOTE (MINECO; CGL 2017-86050-R) and TRAMPA (MINECO; PID 2020-119196RB-C21). C.R C´anovas thanks the Spanish Ministry of Science and Innovation for the Postdoctoral Fellowship granted under application reference RYC 2019- 027949-I. M.D. Basallote thanks the Spanish Ministry of Science and Innovation for the Postdoctoral Fellowship granted under application reference IJC 2018-035056-I. A. Parviainen thanks the Spanish Ministry of Science and Innovation for the Postdoctoral Fellowship granted under application reference IJCI-2016-27412. The comments and helpful criticisms of three anonymous reviewers and the support of Professor Wen-Xiong Wang (Editor) have considerably improved the original manuscript and are also gratefully acknowledged. Funding for open access charge: Universidad de Huelva/CBUA. | This study investigates the behavior of Tl in the Ría de Huelva (SW Spain), one of the most metal polluted estuaries in the world. Dissolved Tl concentration displayed a general decrease across the estuary during the dry season (DS); from 5.0 to 0.34 μg/L in the Tinto and Odiel estuaries, respectively, to 0.02 μg/L in the channel where the rivers join. A slighter decrease was observed during the wet season (WS) (from 0.72 to 0.14 μg/L to 0.02 μg/L) due to the dilution effect of rainfalls in the watersheds. These values are 3 orders of magnitude higher than those reported in other estuaries worldwide. Different increases in Tl concentrations with salinity were observed in the upper reaches of the Tinto and Odiel estuaries, attributed to desorption processes from particulate matter. Chemical and mineralogical evidences of particulate matter, point at Fe minerals (i.e., jarosite) as main drivers of Tl particulate transport in the estuary. Unlike other estuaries worldwide, where a fast sorption process onto particulate matter commonly takes place, Tl is mainly desorbed from particulate matter in the Tinto and Odiel estuaries. Thus, Tl may be released back from jarositic particulate matter across the salinity gradient due to the increasing proportion of unreactive TlCl0 and K+ ions, which compete for adsorption sites with Tl+ at increasing salinities. A mixing model based on conservative elements revealed a 6-fold increase in Tl concentrations related to desorption processes. However, mining spills like that occurred in May 2017 may contribute to enhance dissolved and particulate Tl concentrations in the estuary as well as to magnify these desorption processes (up to around 1100% of Tl release), highlighting the impact of the mine spill on the remobilization of Tl from the suspended matter to the water column. | CAPOTE (MINECO; CGL 2017-86050-R) | TRAMPA (MINECO; PID 2020-119196RB-C21) | Spanish Ministry of Science and Innovation for the Postdoctoral Fellowship granted under application reference RYC 2019- 027949-I. | Postdoctoral Fellowship granted under application reference IJCI-2016-27412 | Funding for open access charge: Universidad de Huelva/CBUA
Показать больше [+] Меньше [-]Short- and long-term effects of decabromodiphenyl ether (BDE-209) on sediment denitrification using a semi-continuous microcosm Полный текст
2022
Wan, Rui | Li, Xiaoxiao | Zha, Yunyi | Zheng, Xiong | Huang, Haining | Li, Minghui
The widespread use of decabromodiphenyl ether (BDE-209) resulted in its deposition in environmental media and biological matrices. However, to date, few studies focused on the effect of BDE-209 on microorganisms, and those available were investigated via an enclosed system completely cutting off the communication between testing system and its native environment. Herein, 4.0 mg/g BDE-209 acute exposure induced a 20% decline of NOX-N (the sum of NO₃⁻–N and NO₂⁻–N) removal efficiency and a significant accumulation of NO₂⁻–N and N₂O. These inhibitory effects presented in a BDE-209 concentration-dependent manner. Using a semi-continuous microcosm, the inhibitory effects of BDE-209 on denitrification were observed to be significantly enhanced with the extending of exposure duration. Denitrifying genes assay illustrated that BDE-209 has an insignificant effect on the global abundance of denitrifying bacteria because of microbial exchange with its overlying water. But the utilization of electron donor (carbon substrate), the activity of electron transport system and denitrifying enzymes were significantly inhibited by BDE-209 exposure in a exposure-duration-dependent manner. Finally, insufficient electron donor and lower efficiency of electron transport and utilization on denitrifying enzymes deteriorated the denitrification performance. These results provided a new insight into BDE-209 influence on denitrification in the natural environment.
Показать больше [+] Меньше [-]Ractopamine at legal residue dosage accelerates atherosclerosis by inducing endothelial dysfunction and promoting macrophage foam cell formation Полный текст
2022
Chen, Chia-Hui | Guo, Bei-Chia | Hu, Po-An | Lee, Hsueh-Te | Hu, Hsuan-Yun | Hsu, Man-Chen | Chen, Wen-Hua | Lee, Tzong-Shyuan
Ractopamine, a synthetic β-adrenoreceptor agonist, is used as an animal feed additive to increase food conversion efficiency and accelerate lean mass accretion in farmed animals. The U.S. Food and Drug Administration claimed that ingesting products containing ractopamine residues at legal dosages might not cause short-term harm to human health. However, the effect of ractopamine on chronic inflammatory diseases and atherosclerosis is unclear. Therefore, we investigated the effects of ractopamine on atherosclerosis and its action mechanism in apolipoprotein E-null (apoe⁻/⁻) mice and human endothelial cells (ECs) and macrophages. Daily treatment with ractopamine for four weeks increased the body weight and the weight of brown adipose tissues and gastrocnemius muscles. However, it decreased the weight of white adipose tissues in apoe⁻/⁻ mice. Additionally, ractopamine exacerbated hyperlipidemia and systemic inflammation, deregulated aortic cholesterol metabolism and inflammation, and accelerated atherosclerosis. In ECs, ractopamine treatment induced endothelial dysfunction and increased monocyte adhesion and transmigration across ECs. In macrophages, ractopamine dysregulated cholesterol metabolism by increasing oxidized low-density lipoprotein (oxLDL) internalization and decreasing reverse cholesterol transporters, increasing oxLDL-induced lipid accumulation. Collectively, our findings revealed that ractopamine induces EC dysfunction and deregulated cholesterol metabolism of macrophages, which ultimately accelerates atherosclerosis progression.
Показать больше [+] Меньше [-]Interplay between arsenic and selenium biomineralization in Shewanella sp. O23S Полный текст
2022
Staicu, Lucian C. | Wójtowicz, Paulina J. | Molnár, Zsombor | Ruiz-Agudo, Encarnación | Gallego, José Luis R. | Baragaño, Diego | Pósfai, Mihály
Bacteria play crucial roles in the biogeochemical cycle of arsenic (As) and selenium (Se) as these elements are metabolized via detoxification, energy generation (anaerobic respiration) and biosynthesis (e.g. selenocysteine) strategies. To date, arsenic and selenium biomineralization in bacteria were studied separately. In this study, the anaerobic metabolism of As and Se in Shewanella sp. O23S was investigated separately and mixed, with an emphasis put on the biomineralization products of this process. Multiple analytical techniques including ICP-MS, TEM-EDS, XRD, Micro-Raman, spectrophotometry and surface charge (zeta potential) were employed. Shewanella sp. O23S is capable of reducing selenate (SeO₄²⁻) and selenite (SeO₃²⁻) to red Se(-S)⁰, and arsenate (AsO₄³⁻) to arsenite (AsO₃³⁻). The release of H₂S from cysteine led to the precipitation of AsS minerals: nanorod AsS and granular As₂S₃. When As and Se oxyanions were mixed, both As–S and Se(-S)⁰ biominerals were synthesized. All biominerals were extracellular, amorphous and presented a negative surface charge (−24 to −38 mV). Kinetic analysis indicated the following reduction yields: SeO₃²⁻ (90%), AsO₄³⁻ (60%), and SeO₄²⁻ (<10%). The mix of SeO₃²⁻ with AsO₄³⁻ led to a decrease in As removal to 30%, while Se reduction yield was unaffected (88%). Interestingly, SeO₄²⁻ incubated with AsO₄³⁻ boosted the Se removal (71%). The exclusive extracellular formation of As and Se biominerals might indicate an extracellular respiratory process characteristic of various Shewanella species and strains. This is the first study documenting a complex interplay between As and Se oxyanions: selenite decreased arsenate reduction, whereas arsenate stimulated selenate reduction. Further investigation needs to clarify whether Shewanella sp. O23S employs multi-substrate respiratory enzymes or separate, high affinity enzymes for As and Se oxyanion respiration.
Показать больше [+] Меньше [-]Community-level and function response of photoautotrophic periphyton exposed to oxytetracycline hydrochloride Полный текст
2022
Wang, Zhenfang | Yin, Sicheng | Chou, Qingchuan | Zhou, Dong | Jeppesen, Erik | Wang, Liqing | Zhang, Wei
Periphyton is considered important for removal of organic pollutants from water bodies, but knowledge of the impacts of antibiotics on the community structure and ecological function of waterbodies remains limited. In this study, the effects of oxytetracycline hydrochloride (OTC) on the communities of photoautotrophic epilithon and epipelon and its effect on nitrogen and phosphorus concentrations in the water column were studied in a 12-day mesocosm experiment. The dynamics of nitrogen and phosphorus concentrations in the epipelon and epilithon experiment showed similar patterns. The concentrations of total nitrogen, dissolved total nitrogen, ammonium nitrogen, total phosphorus and dissolved total phosphorus in the water column increased rapidly during the initial days of exposure, after which a downward trend occurred. In the epilithon experiment, we found that the photosynthesis (Fv/Fm) and biomass of epilithon were significantly (P < 0.05) stimulated in the low concentration group. Contrarily, growth and photosynthesis (Fv/Fm) were significantly (P < 0.05) reduced in the medium and high concentration group. We further found that the photosynthetic efficiency of photoautotrophic epilithon was negatively correlated with the concentrations of nitrogen and phosphorus in the water column (P < 0.05). Principal coordinate analysis (PCoA) showed that the communities of epilithic algae in the control group and in the low concentration group were significantly (P < 0.05) different from that of the high concentration group during the initial 4 days. After 8 days’ exposure, all groups tended to be similar, indicating that epilithon showed rapid adaptability and/or resilience. Similar results were found for the relative abundance of some epilithic algae. Our findings indicate that the biofilm system has strong tolerance and adaptability to OTC as it recovered fast after an initial suppression, thus showing the important role of periphyton in maintaining the dynamic balance of nutrients with other processes in aquatic ecosystems.
Показать больше [+] Меньше [-]Mechanistic insight and bifunctional study of a sulfide Fe3O4 coated biochar composite for efficient As(III) and Pb(II) immobilization in soils Полный текст
2022
Wang, Gehui | Peng, Cheng | T̤āriq, Muḥammad | Lin, Sen | Wan, Jiang | Liang, Weiyu | Zhang, Wei | Zhang, Lehua
Trace elements contamination in soil has aroused global concern nowadays, but the efficient, multifunctional, and economically viable method still remains a major challenge. In this research study, a sulfide Fe₃O₄ coated biochar composite (S/Fe-BC) has been synthesized successfully and applied to As(III)/Pb(II) co-contaminated soil. The immobilization efficiency of S/Fe-BC (2%) for the two elements exceeded 90%, and could ensure the synchronous and efficient immobilization in a wide range of pH (4.0–8.0). The TCLP-As and Pb amounts were sharply dropped after 28 days of stabilization; Meanwhile, a majority of exchangeable and carbonate-bound fractions of As and Pb were transferred into the less accessible residuals. Compared with Fe₃O₄ coated BC, the good immobilization performance of S/Fe-BC was mainly related to the enhancement of specific surface area, improvement of ionic exchange process, followed by the increase of Pb(II) precipitation and As(III) oxidation. Furthermore, competitive and synergistic effects were observed. In depth characterization analyses revealed the simultaneous immobilization mechanisms involving the adsorption, precipitation (Pb(OH)₂, PbSO₄, and PbS), co-precipitation (PbFeAsO₄(OH)), and oxidation. Conclusively, outstanding performance of S/Fe-BC composite is considered as a good multifunctional potential candidate for the immobilization of trace elements from a soil system.
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