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Simultaneous determination of (N-ethyl perfluorooctanesulfonamido ethanol)-based phosphate diester and triester and their biotransformation to perfluorooctanesulfonate in freshwater sediments
2018
Zhang, Shiyi | Peng, Hui | Mu, Di | Zhao, Haoqi | Hu, Jianying
While (N-ethyl perfluorooctanesulfonamido ethanol)-based phosphates (SAmPAPs) have been proposed as a group of perfluorooctanesulfonate (PFOS) precursors, investigation of their occurrence and fate has been limited to SAmPAP diester. In this study, SAmPAP diester and triester were simultaneously determined in freshwater sediment from Taihu Lake using a newly developed UPLC-MS/MS method, and their biotransformation to PFOS in lake sediment was investigated. SAmPAP diester and triester were detected in sediments with a detection frequency of 56% and 88%, and their mean concentrations were 0.24 ± 0.11 ng/g dry weight (dw) and 0.12 ± 0.03 ng/g dw, respectively. The SAmPAP diester/triester ratio in sediment was 1.1 ± 4.2, much lower than that (6.7) observed in the technical product, and the positive correlation was found between the concentrations of SAmPAP diester and PFOS in sediments (r² = 0.45, p = 0.01), suggesting that SAmPAP diester would be biotransformed to PFOS in the lake sediment. The microbial degradation test in the lake sediments further clarified that SAmPAP diester was biodegraded to PFOS, but SAmPAP triester was highly recalcitrant to microbial degradation. This study suggests that the occurrence of SAmPAP diester in freshwater lake sediments may be an important precursor of PFOS.
Show more [+] Less [-]Integrated assessment of persistent toxic substances in sediments from Masan Bay, South Korea: Comparison between 1998 and 2014
2018
Lee, Junghyun | Hong, Seongjin | Kwon, Bong-Oh | Cha, Seung Ah | Jeong, Hee-Dong | Chang, Won Keun | Ryu, Jongseong | Giesy, John P. | Khim, Jong Seong
Complexity of anthropogenic influences on coastal ecosystems necessitates use of an integrated assessment strategy for effective interpretation and subsequent management. In this study a multiple lines of evidence (LOE) approach for sediment assessment, that combined use of chemistry, toxicity, and benthic community structure in the sediment quality triad was used to assess spatiotemporal changes and potential risks of persistent toxic substances (PTSs) in sediments of Masan Bay highlighting “long-term changes” between 1998 and 2014. Specific target objectives encompassed sedimentary PTSs (PAHs, alkylphenols (APs), and styrene oligomers), potential aryl hydrocarbon receptor (AhR; H4IIE-luc assay)- and estrogen receptor (ER; MVLN assay)-mediated activities, and finally several ecological quality (EcoQ) indices of benthic community structure. Concentrations of target PTSs in Masan Bay sediments were generally less by half in 2014 compared to those measured in 1998. Second, AhR-mediated potencies in sediments also decreased during this time interval, whereas ER-mediated potencies increased (+3790%), indicating that there has been substantial ongoing, input of ER agonists over the past 16 years. Potency balance analysis revealed that only 3% and 22% of the AhR- and ER-mediated potencies could be explained by identified known chemicals, such as PAHs and APs, respectively. This result indicated that non-targeted AhR and ER agonists had a considerable presence in the sediments over time. Third, EcoQ indices tended to reflect PTSs contamination in the region. Finally, ratio-to-mean values obtained from the aforementioned three LOEs indicated that quality of sediments from the outer region of the bay had recovery more during the period of 16-years than did the inner region. Overall, the results showed that even with the progress supported by recent efforts from the Korean governmental pollution control, PTSs remain a threat to local ecosystem, especially in the inner region of Masan Bay.
Show more [+] Less [-]A new approach in separating microplastics from environmental samples based on their electrostatic behavior
2018
Felsing, Stefanie | Kochleus, Christian | Buchinger, Sebastian | Brennholt, Nicole | Stock, Friederike | Reifferscheid, Georg
Numerous studies on microplastics (MPs; Ø < 5 mm) in the aquatic environment have been published, but knowledge about the occurrence and ecological risks of MPs is limited. This is in part because current data on the distribution of MPs are comparable only to a limited extent, due to the many different methods of investigation. In addition, sample preparation is often difficult such that standard procedures are lacking. The aim of this work was to simplify the preparation of different kinds of MP samples. Our method makes use of the electrostatic behavior of plastic particles to facilitate their separation from sample matter, with up to 99% of the original sample mass removed without any loss of MPs. To determine the efficacy of this approach, four different materials (quartz sand, freshwater suspended particulate matter, freshwater sediment, and beach sand) were spiked with MPs (size: 0.063–5 mm from the seven most common types of plastics, one bioplastic type, polyethylene fibers, and tire wear. A modified electrostatic metal/plastic separator was used to reduce the sample mass and concentrate the plastics based on their physical separation. The recovery achieved with this method was as high as nearly 100% for each type of material. The method was then tested on plastic particles of different shapes and types isolated from the Rhine River. These were successfully electroseparated from the four materials, which demonstrated the utility of this method. Its advantages include the simplified handling and preparation of different field samples as well as a much shorter processing time, because after the last separation step there is hardly any biological material remaining in the sample fraction.
Show more [+] Less [-]Spatial and temporal trends in poly- and per-fluorinated compounds in the Laurentian Great Lakes Erie, Ontario and St. Clair
2018
Codling, Garry | Sturchio, Neil C. | Rockne, Karl J. | Li, An | Peng, H. | Tse, Timothy J. | Jones, Paul D. | Giesy, John P.
The temporal and spatial trends in sediment of 22 poly- and perfluorinated (PFAS) compounds were investigated in the southern Great Lakes Erie and Ontario as well as Lake St. Clair. Surface concentrations measured by Ponar grab samples indicated a trend for greater concentrations near to urban sites. Mean concentrations ∑22PFAS were 15.6, 18.2 and 19 ng g−1 dm for Lakes St. Clair, Erie and Ontario, respectively. Perfluoro-n-butanoic acid (PFBA) and Perfluoro-n-hexanoic acid (PFHxA) were frequently determined in surface sediment and upper core samples indicating a shift in use patterns. Where PFBA was identified it was at relatively great concentrations typically >10 ng g−1 dm. However as PFBA and PFHxA are less likely to bind to sediment they may be indicative of pore water concentrations Sedimentation rates between Lake Erie and Lake Ontario differ greatly with greater rates observed in Lake Erie. In Lake Ontario, in general concentrations of PFAS observed in core samples closely follow the increase in use along with an observable change due to regulation implementation in the 1970s for water protection. However some of the more water soluble PFAS were observed in deeper core layers than the time of production could account for, indicating potential diffusion within the sediment. Given the greater sedimentation rates in Lake Erie, it was hoped to observe in greater resolution changes since the mid-1990s. However, though some decrease was observed at some locations the results are not clear. Many cores in Lake Erie had clearly observable gas voids, indicative of gas ebullition activity due to biogenic production, there were also observable mussel beds that could indicate mixing by bioturbation of core layers.
Show more [+] Less [-]Pesticide monitoring and ecotoxicological risk assessment in surface water bodies and sediments of a tropical agro-ecosystem
2018
Carazo Rojas, Elizabeth | Pérez-Rojas, Greivin | Pérez-Villanueva, Marta | Chinchilla-Soto, Cristina | Chin-Pampillo, Juan Salvador | Aguilar-Mora, Paula | Alpízar-Marín, Melvin | Masís-Mora, Mario | Rodríguez-Rodríguez, Carlos E. | Vryzas, Zisis
A pesticide monitoring study including 80 and 60 active ingredients (in surface waters and sediments, respectively) was carried out in a river basin in Costa Rica during 2007–2012. A special emphasis was given on the exceptional ecological conditions of the tropical agro-ecosystem and the pesticide application strategies in order to establish a reliable monitoring network. A total of 135 water samples and 129 sediment samples were collected and analyzed. Long-term aquatic ecotoxicological risk assessment based on risk quotient in three trophic levels was conducted. Short-term risk assessment was used to calculate the toxic unit and prioritization of sampling sites was conducted by the sum of toxic units in both aquatic and sediment compartments. Dimethoate (61.2 μg/L), propanil (30.6 μg/L), diuron (22.8 μg/L) and terbutryn (4.8 μg/L) were detected at the highest concentrations in water samples. Carbendazim and endosulfan were the most frequently detected pesticides in water and sediment samples, respectively. Triazophos (491 μg/kg), cypermethrin (71.5 μg/kg), permethrin (47.8 μg/kg), terbutryn (38.7 μg/kg), chlorpyrifos (18.2 μg/kg) and diuron (11.75 μg/kg) were detected at the highest concentrations in sediment samples. The pesticides carbendazim, diuron, endosulfan, epoxyconazole, propanil, triazophos and terbutryn showed non-acceptable risk even when a conservative scenario was considered. Sum TUsite higher than 1 was found for one and two sampling sites in water and sediment compartments, respectively, suggesting high acute toxicity for the ecosystem.Exceptional ecological conditions of the tropical agro-ecosystem affect the fate of pesticides in water and sediment environment differently than the temperate one.
Show more [+] Less [-]Assessment of microplastics derived from mariculture in Xiangshan Bay, China
2018
Chen, Minglong | Jin, Meng | Tao, Peiran | Wang, Zheng | Xie, Weiping | Yu, Xubiao | Wang, Kan
Mariculture activities including enclosure, raft and cage cultures employ a variety of plastic gear such as fishing nets, buoyant material and net cages. The plastic gear poses a potential source of microplastics to the coastal environment, but relevant data on the impacts of mariculture are still limited. To this end, a semi-enclosed narrow bay (i.e., Xiangshan Bay, China) with a long-term mariculture history was investigated to assess how mariculture activities affect microplastics in seawater and sediment. The results indicated that mariculture-derived microplastics accounted for approximately 55.7% and 36.8% of the microplastics in seawater and sediment, respectively. The average microplastic abundances of seawater and sediment were 8.9 ± 4.7 (mean ± SD, n = 18) items/m³ seawater and 1739 ± 2153 (n = 18) items/kg sediment, respectively. The types of mariculture-derived microplastics included polyethylene (PE) foam, PE nets, PE film, polypropylene (PP) rope, polystyrene (PS) foam and rubber. PE foam had the highest proportion (38.6%) in the seawater samples. High usage rates and the porous structure of PE foam led to the high abundance. The average microplastic sizes of seawater and sediment are 1.54 ± 1.53 mm and 1.33 ± 1.69 mm, respectively. The spatial variations in the abundance and size of microplastics implied that the mariculture-derived microplastics in Xiangshan Bay were transported along the Bay to the open sea. The results of this study indicate that mariculture activity can be a significant source of microplastics. Further research is required to investigate how the high microplastic abundance in mariculture zone affects marine organisms, especially cultured seafood.
Show more [+] Less [-]Seasonal and spatial distribution of antibiotic resistance genes in the sediments along the Yangtze Estuary, China
2018
Guo, Xing-pan | Liu, Xinran | Niu, Zuo-shun | Lu, Da-pei | Zhao, Sai | Sun, Xiao-li | Wu, Jia-yuan | Chen, Yu-ru | Tou, Fei-yun | Hou, Lijun | Liu, Min | Yang, Yi
Antibiotics resistance genes (ARGs) are considered as an emerging pollutant among various environments. As a sink of ARGs, a comprehensive study on the spatial and temporal distribution of ARGs in the estuarine sediments is needed. In the present study, six ARGs were determined in sediments taken along the Yangtze Estuary temporally and spatially. The sulfonamides, tetracyclines and fluoroquinolones resistance genes including sul1, sul2, tetA, tetW, aac(6’)-Ib, and qnrS, were ubiquitous, and the average abundances of most ARGs showed significant seasonal differences, with relative low abundances in winter and high abundances in summer. Moreover, the relative high abundances of ARGs were found at Shidongkou (SDK) and Wusongkou (WSK), which indicated that the effluents from the wastewater treatment plant upstream and inland river discharge could influence the abundance of ARGs in sediments. The positive correlation between intI1 and sul1 implied intI1 may be related to the occurrence and propagation of sulfonamides resistance genes. Correlation analysis and redundancy discriminant analysis showed that antibiotic concentrations had no significant correlation to their corresponding ARGs, while the total extractable metal, especially the bioavailable metals, as well as other environmental factors including temperature, clay, total organic carbon and total nitrogen, could regulate the occurrence and distribution of ARGs temporally and spatially. Our findings suggested the comprehensive effects of multiple pressures on the distribution of ARGs in the sediments, providing new insight into the distribution and dissemination of ARGs in estuarine sediments, spatially and temporally.
Show more [+] Less [-]Distribution and potential ecological risk of 50 phenolic compounds in three rivers in Tianjin, China
2018
Zhong, Wenjue | Wang, Donghong | Wang, Zijian
Phenolic compounds widely exist in the surface water of many countries; however, few studies have simultaneously analyzed and evaluated broad-spectrum phenolic compounds in various components of the water environment. Therefore this study analyzed the distribution and potential ecological risk of 50 phenolic compounds in the surface water, sediment and suspended particulate matter of three important rivers in Tianjin, the main heavy industry city with high pollution in China. The qualitative results show that phenolic pollution existed extensively in the three rivers and the kinds of phenolic compounds in the water were relatively higher than in both sediment and suspended particulate matter. The quantitative results show that the phenolic pollution in the wet-season samples was serious than dry-season samples. Meanwhile, total concentrations of phenolic compounds in three components from the Dagu Drainage River (DDR) were all much higher than those in the Beitang Drainage River (BDR) and Yongdingxin River (YDXR). The highest total concentrations of phenolic compounds in three components all appeared in wet-season samples in DDR, and the highest total concentration was 1354 μg/L in surface water, 719 μg/kg dw in suspended particulate matter and 2937 μg/kg dw in sediment, respectively. The ecological risk of phenolic compounds in surface water was evaluated using the quotient method, and phenolic compounds with risk quotient (RQ) > 1 (RQ > 0.3 for YDXR) were identified as priority pollutants. Five kinds of phenolic compounds were identified as priority phenolic compounds in BDR, and the order of risk was 2-cresol > 2,4-xylenol > 2-sec-butylphenol > 2-naphthol > 3-cresol. Six kinds of phenolic compounds were identified as priority phenolic compounds in DDR, and the order of risk was 2-naphthol > p-chloro-m-xylenol > 4-cresol > 3-cresol > 2,4-xylenol > 2,3,6-Trimethylphenol. In YDXR, only phenol, 2-naphthol and 2,4-xylenol were identified as priority phenolic compounds.
Show more [+] Less [-]Distribution and ecotoxicological state of phthalate esters in the sea-surface microlayer, seawater and sediment of the Bohai Sea and the Yellow Sea
2018
Zhang, Ze-Ming | Zhang, Hong-Hai | Zou, Ya-Wen | Yang, Gui-Peng
The spatial distribution, chemical composition and ecological risk of 16 phthalate esters (PAEs) were investigated in the sea-surface microlayer (SML), seawater and sediment samples of the Bohai Sea (BS) and the Yellow Sea (YS). The concentration levels of the ΣPAEs spanned a range of 449–13441 ng L−1 in the SML, 453–5108 ng L−1 in seawater, and 1.24–15.8 mg kg−1 in the sediment samples, respectively, with diisobutyl phthalate (DiBP), di-n-butyl phthalate (DBP) and di-ethylhexyl phthalate (DEHP) as the dominant PAEs in both the water and sediment samples. The concentrations of ΣPAEs in the BS were higher than those in the YS. The vertical distribution of ΣPAEs in the water column showed that the concentrations were higher in the surface waters, but decreased slightly with depth, and started to increase at the bottom. Additionally, PAEs were significantly enriched in the SML, with an average enrichment factor of 1.46. The ecological risk of the PAEs was evaluated by the risk quotient (RQ) method, which indicated that DEHP posed a high risk to aquatic organisms in the whole water-phase, while the RQ values of DBP and DiBP reached a high risk levels in sedimentary environment.
Show more [+] Less [-]Bioavailability and uptake of smelter emissions in freshwater zooplankton in northeastern Washington, USA lakes using Pb isotope analysis and trace metal concentrations
2018
Child, A.W. | Moore, B.C. | Vervoort, J.D. | Beutel, M.W.
The upper Columbia River and associated valley systems are highly contaminated with metal wastes from nearby smelting operations in Trail, British Columbia, Canada (Teck smelter), and to a lesser extent, Northport, Washington, USA (Le Roi smelter). Previous studies have investigated depositional patterns of airborne emissions from these smelters, and documented the Teck smelter as the primary metal contamination source. However, there is limited research directed at whether these contaminants are bioavailable to aquatic organisms. This study investigates whether smelter derived contaminants are bioavailable to freshwater zooplankton. Trace metal (Zn, Cd, As, Sb, Pb and Hg) concentrations and Pb isotope compositions of zooplankton and sediment were measured in lakes ranging from 17 to 144 km downwind of the Teck smelter. Pb isotopic compositions of historic ores used by both smelters are uniquely less radiogenic than local geologic formations, so when zooplankton assimilate substantial amounts of smelter derived metals their compositions deviate from local baseline compositions toward ore compositions. Sediment metal concentrations and Pb isotope compositions in sediment follow significant (p < 0.001) negative exponential and sigmoidal patterns, respectively, as distance from the Teck smelting operation increases. Zooplankton As, Cd, and Sb contents were related to distance from the Teck smelter (p < 0.05), and zooplankton Pb isotope compositions suggest As, Cd, Sb and Pb from historic and current smelter emissions are biologically available to zooplankton. Zooplankton from lakes within 86 km of the Teck facility display isotopic evidence that legacy ore pollution is biologically available for assimilation. However, without water column data our study is unable to determine if legacy contaminants are remobilized from lake sediments, or erosional pathways from the watershed.
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