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PAH distributions in sediments in the oil sands monitoring area and western Lake Athabasca: Concentration, composition and diagnostic ratios
2016
Evans, Marlene | Davies, Martin | Janzen, Kim | Muir, Derek | Hazewinkel, Rod | Kirk, Jane | de Boer, Dirk
Oil sands activities north of Fort McMurray, Alberta, have intensified in recent years with a concomitant debate as to their environmental impacts. The Regional Aquatics Monitoring Program and its successor, the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring (JOSM), are the primary aquatic programs monitoring this industry. Here we examine sediment data (collected by Ekman grabs) to investigate trends and sources of polycyclic aromatic hydrocarbons (PAHs), supplementing these data with sediment core studies. Total PAH (ΣPAH) concentrations were highest at Shipyard Lake (6038 ± 2679 ng/g) in the development center and lower at Isadore's Lake (1660 ± 777 ng/g) to the north; both lakes are in the Athabasca River Valley and lie below the developments. ΣPAH concentrations were lower (622–930 ng/g) in upland lakes (Kearl, McClelland) located further away from the developments. ΣPAH concentrations increased at Shipyard Lake (2001–2014) and the Ells River mouth (1998–2014) but decreased in nearshore areas at Kearl Lake (2001–2014) and a Muskeg River (2000–2014) site. Over the longer term, ΣPAH concentrations increased in Kearl (1934–2012) and Sharkbite (1928–2010) Lakes. Further (200 km) downstream in the Athabasca River delta, ΣPAH concentrations (1029 ± 671 ng/g) increased (1999–2014) when %sands were included in the regression model; however, 50 km to the east, concentrations declined (1926–2009) in Lake Athabasca. Ten diagnostic ratios based on anthracene, phenanthrene, fluoranthene, pyrene, benz[a]anthracene, chrysene, indeno[123-cd]pyrene, dibenz[a,h]anthracene, dibenzothiophene and retene were examined to infer spatial and temporal trends in PAH sources (e.g., combustion versus petrogenic) and weathering. There was some evidence of increasing contributions of unprocessed oil sands and bitumen dust to Shipyard, Sharkbite, and Isadore's Lakes and increased combustion sources in the Athabasca River delta. Some CCME interim sediment quality guidelines were exceeded, primarily in Shipyard Lake and near presumed natural bitumen sources.
Show more [+] Less [-]Polybrominated diphenyl ethers (PBDEs) and alternative brominated flame retardants (aBFRs) in sediments from four bays of the Yellow Sea, North China
2016
Zhen, Xiaomei | Tang, Jianhui | Xie, Zhiyong | Wang, Runmei | Huang, Guopei | Zheng, Qian | Zhang, Kai | Sun, Yongge | Tian, Chongguo | Pan, Xiaohui | Li, Jun | Zhang, Gan
The distribution characteristics and potential sources of polybrominated diphenyl ethers (PBDEs) and alternative brominated flame retardants (aBFRs) were investigated in 54 surface sediment samples from four bays (Taozi Bay, Sishili Bay, Dalian Bay, and Jiaozhou Bay) of North China's Yellow Sea. Of the 54 samples studied, 51 were collected from within the four bays and 3 were from rivers emptying into Jiaozhou Bay. Decabromodiphenylethane (DBDPE) was the predominant flame retardant found, and concentration ranged from 0.16 to 39.7 ng g−1 dw and 1.13–49.9 ng g−1 dw in coastal and riverine sediments, respectively; these levels were followed by those of BDE 209, and its concentrations ranged from n.d. to 10.2 ng g−1 dw and 0.05–7.82 ng g−1 dw in coastal and riverine sediments, respectively. The levels of DBDPE exceeded those of decabromodiphenyl ether (BDE 209) in most of the samples in the study region, whereas the ratio of DBDPE/BDE 209 varied among the four bays. This is indicative of different usage patterns of brominated flame retardants (BFRs) and also different hydrodynamic conditions among these bay areas. The spatial distribution and composition profile analysis indicated that BFRs in Jiaozhou Bay and Dalian Bay were mainly from local sources, whereas transport from Laizhou Bay by coastal currents was the major source of BFRs in Taozi Bay and Sishili Bay. Both the ∑PBDEs and ∑aBFRs (sum of pentabromotoluene (PBT), 2,3-diphenylpropyl-2,4,6-tribromophenyl ether (DPTE), pentabromoethylbenzene (PBEB), and hexabromobenzene (HBB)) were at low concentrations in all the sediments. This is probably attributable to a combination of factors such as low regional usage of these products, atmospheric deposition patterns, coastal currents transportation patterns, and degradation processes for higher BDE congeners. This paper is the first study that has investigated the levels of DBDPE in the coastal sediments of China's Yellow Sea.
Show more [+] Less [-]Occurrence, distribution and source apportionment of polychlorinated naphthalenes (PCNs) in sediments and soils from the Liaohe River Basin, China
2016
Li, Fang | Jin, Jing | Gao, Yuan | Geng, Ningbo | Tan, Dongqin | Zhang, Haijun | Ni, Yuwen | Chen, Jiping
The occurrence and spatial distribution of polychlorinated naphthalenes (PCNs) were investigated in sediments, upland and paddy soils from the Liaohe River Basin. Concentrations of ΣPCNs were in the range of 0.33–12.49 ng g⁻¹ dry weight (dw) in sediments and 0.61–6.60 ng g⁻¹ dw in soils, respectively. Tri-CNs and tetra-CNs were the dominating homologues. An increasing trend of PCNs contamination was found in sediments with the rivers flowing through industrial areas and cities. Soils collected near cities exhibited higher abundance of PCNs than that of rural areas. The distribution of PCNs was related to the local industrial activities, rather than total organic carbon. Positive matrix factorization (PMF) was used for the source apportionment of PCNs in sediments and paddy soils. The result of PMF indicated that PCNs in sediments and paddy soils were mainly from the industrial processes, with additional contributions from the historical use of Halowax 1014 and atmospheric deposition.
Show more [+] Less [-]Shared effects of organic microcontaminants and environmental stressors on biofilms and invertebrates in impaired rivers
2016
Sabater, S. | Barceló, D. | De Castro-Català, N. | Ginebreda, A. | Kuzmanovic, M. | Petrovic, M. | Picó, Y. | Ponsatí, L. | Tornés, E. | Muñoz, I.
Land use type, physical and chemical stressors, and organic microcontaminants were investigated for their effects on the biological communities (biofilms and invertebrates) in several Mediterranean rivers. The diversity of invertebrates, and the scores of the first principal component of a PCA performed with the diatom communities were the best descriptors of the distribution patterns of the biological communities against the river stressors. These two metrics decreased according to the progressive site impairment (associated to higher area of agricultural and urban-industrial, high water conductivity, higher dissolved organic carbon and dissolved inorganic nitrogen concentrations, and higher concentration of organic microcontaminants, particularly pharmaceutical and industrial compounds). The variance partition analyses (RDAs) attributed the major share (10%) of the biological communities' response to the environmental stressors (nutrients, altered discharge, dissolved organic matter), followed by the land use occupation (6%) and of the organic microcontaminants (2%). However, the variance shared by the three groups of descriptors was very high (41%), indicating that their simultaneous occurrence determined most of the variation in the biological communities.
Show more [+] Less [-]Source apportionment of trace metals in river sediments: A comparison of three methods
2016
Chen, Haiyang | Teng, Yanguo | Li, Jiao | Wu, Jin | Wang, Jinsheng
Increasing trace metal pollution in river sediment poses a significant threat to watershed ecosystem health. Identifying potential sources of sediment metals and apportioning their contributions are of key importance for proposing prevention and control strategies of river pollution. In this study, three advanced multivariate receptor models, factor analysis with nonnegative constraints (FA-NNC), positive matrix factorization (PMF), and multivariate curve resolution weighted-alternating least-squares (MCR-WALS), were comparatively employed for source apportionment of trace metals in river sediments and applied to the Le'an River, a main tributary of Poyang Lake which is the largest freshwater lake in China. The pollution assessment with contamination factor and geoaccumulation index suggested that the river sediments in Le'an River were contaminated severely by trace metals due to human activities. With the three apportionment tools, similar source profiles of trace metals in sediments were extracted. Especially, the MCR-WALS and PMF models produced essentially the same results. Comparatively speaking, the weighted schemes might give better solutions than the unweighted FA-NNC because the uncertainty information of environmental data was considered by PMF and MCR-WALS. Anthropogenic sources were apportioned as the most important pollution sources influencing the sediment metals in Le'an River with contributions of about 90%. Among them, copper tailings occupied the largest contribution (38.4–42.2%), followed by mining wastewater (29.0–33.5%), and agricultural activities (18.2–18.7%). To protect the ecosystem of Le'an River and Poyang Lake, special attention should be paid to the discharges of mining wastewater and the leachates of copper tailing ponds in that region.
Show more [+] Less [-]Comparison of pollution indices for the assessment of heavy metal in Brisbane River sediment
2016
Duodu, Godfred Odame | Goonetilleke, Ashantha | Ayoko, G. A. (Godwin A.)
Estuarine environment is complex and receives different contaminants from numerous sources that are persistent, bioaccumulative and toxic. The distribution, source, contamination and ecological risk status of heavy metals in sediment of Brisbane River, Australia were investigated. Sediment samples were analysed for major and minor elements using LA-ICP-MS. Principal component analysis and cluster analysis identified three main sources of metals in the samples: marine sand intrusion, mixed lithogenic and sand intrusion as well as transport related. To overcome inherent deficiencies in using a single index, a range of sediment quality indices, including contamination factor, enrichment factor, index of geo-accumulation, modified degree of contamination, pollution index and modified pollution index were utilised to ascertain the sediment quality. Generally, the sediment is deemed to be “slightly” to “heavily” polluted. A further comparison with the Australian Sediment Quality Guidelines indicated that Ag, Cr, Cu, Ni, Pb and Zn had the potential to rarely cause biological effects while Hg could frequently cause biological effects. Application of potential ecological risk index (RI) revealed that the sediment poses moderate to considerable ecological risk. However, RI could not account for the complex sediment behaviour because it uses a simple contamination factor. Consequently, a modified ecological risk index (MRI) employing enrichment factor is proposed. This provides a more reliable understanding of whole sediment behaviour and classified the ecological risk of the sediment as moderate to very high. The results demonstrate the need for further investigation into heavy metal speciation and bioavailability in the sediment to ascertain the degree of toxicity.
Show more [+] Less [-]Sterol ratios as a tool for sewage pollution assessment of river sediments in Serbia
2016
Matić Bujagić, Ivana | Grujić, Svetlana | Jauković, Zorica | Laušević, Mila
In this work, source pollution tracing of the sediments of the Danube River and its tributaries in Serbia was performed using sterol ratios. Improved liquid chromatography-tandem mass spectrometry method, which enabled complete chromatographic separation of four analytes with identical fragmentation reactions (epicoprostanol, coprostanol, epicholestanol and cholestanol), was applied for the determination of steroid compounds (hormones, human/animal and plant sterols). A widespread occurrence of sterols was identified in all analyzed samples, whereas the only detected hormones were mestranol and 17α-estradiol. A human-sourced sewage marker coprostanol was detected at the highest concentration (up to 1939 ng g−1). The ratios between the key sterol biomarkers, as well as the percentage of coprostanol relative to the total sterol amount, were applied with the aim of selecting the most reliable for distinction between human-sourced pollution and the sterols originated from the natural sources in river sediments. The coprostanol/(cholesterol + cholestanol) and coprostanol/epicoprostanol ratios do not distinguish between human and natural sources of sterols in the river sediments in Serbia. The most reliable sterol ratios for the sewage pollution assessment of river sediments in the studied area were found to be coprostanol/(coprostanol + cholestanol), coprostanol/cholesterol and epicoprostanol/coprostanol. For the majority of sediments, human-derived pollution was determined. Two sediment samples were identified as influenced by a combination of human and natural biogenic sources.
Show more [+] Less [-]Polychlorinated biphenyls (PCBs) in sediments/soils of different wetlands along 100-year coastal reclamation chronosequence in the Pearl River Estuary, China
2016
Zhao, Qingqing | Bai, Junhong | Lu, Qiongqiong | Gao, Zhaoqin | Jia, Jia | Cui, Baoshan | Liu, Xinhui
PCBs (polychlorinated biphenyls) were determined in sediment/soil profiles to a depth of 30 cm from three different wetlands (i.e., ditch wetlands, riparian wetlands and reclaimed wetlands) of the Pearl River Estuary to elucidate their levels, distribution and toxic risks along a 100-year chronosequence of reclamation. All detected PCB congeners and the total 15 PCBs (∑15 PCBs) decreased with depth along sediment/soil profiles in these three wetlands. The ∑15 PCBs concentrations ranged from 17.68 to 169.26 ng/g in surface sediments/soils. Generally, old wetlands tended to have higher PCB concentrations than younger ones. The dominant PCB congeners at all sampling sites were light PCB homologues (i.e., tetra-CBs and tri-CBs). According to the sediment quality guideline, the average PCB concentrations exceeded the threshold effects level (TEL, 21.6 ng/g) at most of the sampling sites, exhibiting possible adverse biological effects, which were dominantly caused by light PCB congeners. The total toxic equivalent (TEQ) concentrations of 10 dioxin-like PCBs (DL-PCBs) detected at all sampling sites ranged from 0.04 to 852.7 (10−3 ng/g), mainly affected by PCB126. Only DL-PCB concentrations in ditch and riparian wetland sediments with 40-year reclamation histories (i.e., D40 and Ri40) exhibited moderate adverse biological effects according to SQGQ values. Principal component analysis indicated that PCBs in three wetland sediments/soils mainly originated from Aroclor 1016, 1242, and 1248. Correlation analysis showed that sediment/soil organic carbon content had a significant correlation with the concentrations of several PCB congeners (P < 0.05), whereas no significant correlations were observed between any PCBs congeners and grain size or aggregate content (P > 0.05).
Show more [+] Less [-]Occurrence and distribution of perfluoroalkyl substances (PFASs) in surface water and bottom water of the Shuangtaizi Estuary, China
2016
Shao, Mihua | Ding, Guanghui | Zhang, Jing | Wei, Lie | Xue, Huanhuan | Zhang, Nannan | Li, Yang | Chen, Guanqun | Sun, Yeqing
Perfluoroalkyl substances (PFASs) have been recognized as emerging environmental pollutants. However, there is limited information on the contamination level and spatial distribution of PFASs in the Shuangtaizi Estuary, where the Shuangtaizi Hekou Nature Reserve is located. In the present study, the contamination level and spatial distribution of PFASs in surface water (approximately 0.5 m below the surface) and bottom water (about 0.5 m above the bottom) of the Shuangtaizi Estuary were investigated. The data indicated that the Shuangtaizi Estuary was commonly contaminated by PFASs. The total concentration of PFASs in surface and bottom water of the Shuangtaizi Estuary ranged from 66.2 to 185 ng L−1 and from 44.8 to 209 ng L−1, respectively. The predominant PFASs were perfluorobutanoic acid (PFBA), perfluoropentanoic acid, perfluorooctanoic acid, perfluorohexanoic acid and perfluorobutane sulfonate (PFBS). In general, PFAS concentrations in surface water samples were lower than those in bottom water samples. The spatial distribution of PFASs in the Shuangtaizi Estuary was mainly affected by particular landform, tide and residual currents in Liaodong Bay. The total mass flux of 15 PFASs from the Shuangtaizi River to Liaodong Bay was estimated to be 352 kg year−1, which was lower than the total flux from the Daling River and the Daliao River. As short-chain PFASs, such as PFBS and PFBA, have been the prevalent compounds in some places and are continuously produced and used, long-term monitoring and effective pollution controls are suggested.
Show more [+] Less [-]Predictors of pesticide concentrations in freshwater trout – The role of life history
2016
Scholes, Rachel C. | Hageman, Kimberly J. | Closs, Gerry | Stirling, Claudine H. | Reid, Malcolm R. | Gabrielsson, Rasmus | Augspurger, Jason M.
Concentrations of halogenated pesticides in freshwater fish can be affected by age, size, trophic position, and exposure history. Exposure history may vary for individual fish caught at a single location due to different life histories, e.g. they may have hatched in different tributaries before migrating to a specific lake. We evaluated correlations of pesticide concentrations in freshwater brown trout (Salmo trutta) from the Clutha River, New Zealand, with potential predictors including capture site, age, length, trophic level, and life history. Life history was determined from otolith (fish ear bone) strontium isotope signatures, which vary among tributaries in the region of our study. Variability in pesticide concentrations between individual fish was not well explained by capture site, age, length, or trophic level. However, hexachlorobenzene (HCB) and chlorpyrifos concentrations were distinct in lake-based trout with different life histories. Additionally, one of the riverine life histories was associated with relatively high concentrations of total endosulfans. Linear models that included all potential predictor variables were evaluated and the resulting best models for HCB, chlorpyrifos, and total endosulfans included life history. These findings show that in cases where otolith isotope signatures vary geographically, they can be used to help explain contaminant concentration variations in fish caught from a single location.
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