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ABSTRACT: A new method using ultrasonic extraction and solid phase extraction (SPE) clean-up pretreatments was developed for the analysis of mono-, di- and tri-substituted polyfluoroalkyl phosphates (abbreviated as mono-PAPs, di-PAPs and tri-PAPs) and perfluorinated phosphonic acids (PFPAs) in sludge from wastewater treatment plants (WWTPs). For the ultrasonic extraction of three mono-PAPs, three di-PAPs and three PFPAs in sludge samples, a mixture of tetrahydrofuran/acetic acid (1:1, v/v) was found to be the most suitable extraction solvent. The subsequently optimized clean-up and enrichment procedures were carried out with weak anion exchange (WAX) cartridges in-line coupled with graphitized carbon black (ENVI-Carb) tubes. Two tri-PAPs were ultrasonically extracted by acetonitrile/tetrahydrofuran (1:1, v/v) and cleaned by mixed-mode anion exchange (MAX) in-line coupled with ENVI-Carb cartridges. The analytes were analyzed by optimized high performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS) method either in negative or positive ionization mode. The method quantification limits (MQLs) of the 11 analytes in sludge ranged from 0.6 to 5.1ng/g, meanwhile the total recoveries of the pretreatment varied from 24% (6:2 mono-PAP) to 107% (PFDPA). The method was successfully applied to analyze 16 sewage sludge samples collected from seven provinces in China, and two mono-PAPs were identified with concentrations ranging from <MQLs to 10.7ng/g.
Talanta 07/2013; 111C:170-7. · 3.79 Impact Factor
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ABSTRACT: Characterization of mercury binding protein in the human body is very important for understanding the metabolism and the mechanism of toxication of ingested mercuric compounds. In this study, mercury-containing protein in human plasma was separated by on-line heart-cutting two-dimensional high performance liquid chromatography (2D-HPLC). This 2D separation system used size exclusion liquid chromatography (SEC) followed by weak anion exchange liquid chromatography (WAX) and the two LC parts were coupled by a six-port valve equipped with a storage loop and controled by the computer. The WAX effluent was determined by both UV detection and inductively coupled plasma-mass spectrometry (ICP-MS) to locate the mercury-containing protein. A unique mercury-containing protein fraction was obtained by 2D-HPLC separation and subsequently identified by HPLC coupled with linear ion trap-Fourier transform ion cyclotron resonance mass spectrometry (HPLC-LTQ-FT). The database search confirmed that the mercury-containing protein in the human plasma is human serum albumin (HSA). The stoichiometry and thermodyamics interaction of inorganic mercury (Hg(2+)) with HSA was studied by isothermal titration calorimetry (ITC) and two binding types were observed. Mercury-containing protein in human plasma was separated and identified in the present study and it is important for understanding the metabolism of mercury in the human body.
Metallomics 06/2013; · 3.90 Impact Factor
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Guangbo Qu,
Sijin Liu,
Shuping Zhang,
Lei Wang,
Xiaoyan Wang,
Bingbing Sun,
Nuoya Yin,
Xiang Gao,
Tian Xia,
Jane-Jane Chen, Guibin Jiang
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ABSTRACT: Graphene and graphene-based nanomaterials display novel and beneficial chemical, electrical, mechanical, and optical characteristics, which endow these nanomaterials with promising applications in a wide spectrum of areas such as electronics and biomedicine. However, its toxicity on health remains unknown and is of great concern. In the present study, we demonstrated that graphene oxide (GO) induced necrotic cell death to macrophages. This toxicity is mediated by activation of toll-like receptor 4 (TLR4) signaling and subsequently in part via autocrine TNF-α production. Inhibition of TLR4 signaling with a selective inhibitor prevented cell death nearly completely. Furthermore, TLR4-deficient bone marrow-derived macrophages were resistant to GO-triggered necrosis. Similarly, GO did not induce necrosis of HEK293T/TLR4-null cells. Macrophagic cell death upon GO treatment was partially attributed to RIP1-RIP3 complex-mediated programmed necrosis downstream of TNF-α induction. Additionally, upon uptake into macrophages, GO accumulated primarily in cytoplasm causing dramatic morphologic alterations and a significant reduction of the macrophagic ability in phagocytosis. However, macrophagic uptake of GO may not be required for induction of necrosis. GO exposure also caused a large increase of intracellular reactive oxygen species (ROS), which contributed to the cause of cell death. The combined data reveal that interaction of GO with TLR4 is the predominant molecular mechanism underlying GO-induced macrophagic necrosis; also, cytoskeletal damage and oxidative stress contribute to decreased viability and function of macrophages upon GO treatment.
ACS Nano 06/2013; · 10.77 Impact Factor
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ABSTRACT: Enhanced regulations, centralized dismantling processes and sophisticated recycling technologies have been implemented in some e-waste dismantling areas in China with regards to environmental and economic aspects since 2005. In this study, rice grain samples were collected from 2006 to 2010 in an e-waste dismantling area to investigate the temporal trends and spatial distribution of As, Cd, Cu and Pb. Geometric means of As, Cd, Cu and Pb in rice samples from the e-waste dismantling area were 111, 217, 4676 and 237 ng g-1, respectively. Levels of Pb showed a significant decreasing trend during the sampling period, whereas the other three elements remained relatively constant or even increasing. Concentrations of Cd, Cu and Pb in e-waste dismantling area were significantly higher than those in non e-waste dismantling area (p<0.05), which showed a close connection between e-waste dismantling activities and elevated Pb, Cu and Cd contents. Risk assessment for human via rice consumption indicated that over 60% of the hazard quotient of Cd exceeded 1 in the e-waste dismantling area. Our study implied that stricter implementation of regulatory measures might lead to positive effects in controlling the release of some heavy metals to the environment. However, environmental behaviors differed with geochemical characteristics of individual elements. Further remediation actions to reduce heavy metal pollution to the surrounding environment might still be needed.
Environmental Science & Technology 05/2013; · 4.80 Impact Factor
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ABSTRACT: Functionalization is an important technique to increase the solubility and biocompatibility of single-wall carbon nanotubes (SWCNTs). In this study, we investigated the cytotoxicity of four types of SWCNTs functionalized with hydroxyl, amino, carboxyl and polyethyleneglycol on MCF7 cells. These functionalized SWCNTs (f-SWCNTs) have insignificant effects on mitochondrial activity and ROS production in MCF7 cells at all test concentrations. However, explicit results revealed that all the tested f-SWCNTs could cause changes of cell morphology, induce cell membrane damage, decrease cell adhesion, and increase cell apoptosis. Therefore, this study shows the potential side effects of f-SWCNTs accompanying with the increase of dispersibility and stability in environment or serum (to prevent their aggregation), and highlights the need for further research to examine the potential toxicity of f-SWCNTs before they are used in the environmental and biomedical fields.
Chemosphere 05/2013; · 3.21 Impact Factor
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ABSTRACT: We demonstrate here a simple one-pot approach to directly fabricate hierarchical hollow anatase TiO2 spheres with a mesoporous shell architecture, which show improved visible light photocatalytic activity owing to their unique structure.
Dalton Transactions 05/2013; · 3.84 Impact Factor
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ABSTRACT: In this paper, multiple proxies of terrestrial organic matters (TOM) were introduced to study the migration behaviors of short chain chlorinated paraffins (SCCPs) in the coastal East China Sea (ECS). The contents of SCCPs in the surface sediment collected from Changjiang (Yangtze) River Delta (CRD) and along the Zhejiang-Fujian coastline ranged from 9.0 to 37.2 ng/g (dry weight, d.w.), displaying a "Band-Style" distribution trend. Spatial distribution patterns of SCCP congeners presented an increasing trend seaward and southward along the coastline for shorter carbon length (C10+C11) and lower chlorinated (Cl5+Cl6+Cl7) congeners, suggesting a spreading tendency seaward and southward from the CRD and the north of the inner shelf. The significant relationship between ΣSCCPs and total organic carbons (TOC) (r2 = 0.402, p < 0.05) indicated that the migration of SCCPs in sediments was markedly affected by TOC. The spatial patterns of the TOM proxies of TOC δ13C, the contents of ΣC27+C29+C31 n-alkanes, Terrestrial Marine Biomarker Ratio (TMBR) and terrestrial TOC (T-TOC) were all similar to that of ΣSCCPs. Linear relationships between SCCP contents and both the contents of ΣC27+C29+C31 n-alkanes (r2 = 0.537, p < 0.05) and T-TOC (r2 = 0.495, p < 0.05) were also observed. The consistence demonstrated that a major portion of sedimentary SCCPs in the coastal ECS should be from the river input of Changjiang River (CR) and deposited in the CRD and along the inner shelf of the ECS, but only a minor fraction was transported to the offshore areas.
Environmental Science & Technology 04/2013; · 4.80 Impact Factor
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ABSTRACT: Nanosilver (nAg) is a considerably important nanomaterial due to its unique physical and chemical features and its intrinsic antimicrobial properties. Thus far, nAg has been widely applied in a variety of fields including biomedicine. Considering the safety and adverse influence, investigations into the biological fate and potential toxicity of nAg are essential for its safe and appropriate applications. In the current study, we exposed nAg to BALB/c mice at various concentrations via intraperitoneal (IP) and intravenous (IV) routes. The results showed that nAg was predominantly localized in liver and spleen in mice for both administration methods. Compared to IP administration, nAg was quickly removed and excreted from body with IV administration. The accumulation of nAg in livers caused remarkable hepatic toxicity. For the first time, we demonstrated that nAg had the ability to cross the placental barrier and accumulate in fetuses. Furthermore, the results of nAg tissue distribution in male mice revealed that nAg could pass through the blood-testis barrier, resulting in localization in testis. Additionally, the pharmacokinetic process of nAg in mice was also assessed in this study. Our findings indicated that nAg retention in mouse body could last for more than 4 months, and the silver content in the major recipient organs decreased in a time-dependent manner. Taken together, these results would be of great assistance in clarifying the safety issue of nAg as drug delivery and therapeutic agent, and in the understanding of the mechanisms underlying nAg-meditated toxicity.
Current pharmaceutical design 04/2013; · 4.41 Impact Factor
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ABSTRACT: Chronic exposure to arsenic (As) threatens human health. To systematically understand the health risks induced by As ingestion, we explored water and diet contributions to As exposure, and compared As in biomarkers and the arsenicosis in a geogenic As area in China. In this study, high percentages of water (77% of n=131 total samples), vegetables (92%, n=120), cereals (32%, n=25), urine (70%, n=99), nails (76%, n=176), and hair (62%, n=61) contained As higher than the acceptable levels. Dietary As contributed 92% of the average daily dose (ADD) when the water As concentration was less than 10 μg/L, for which 5 out of 30 examined participants were diagnosed with arsenicosis symptoms. The distinct positive correlation between ADD and As concentrations in urine, nails, and hair suggests different applicability for these biomarkers. Methylated As as the predominant urinary As species confirms that the ingested inorganic As is methylated and is excreted through urine. In situ micro-distribution and speciation analysis indicate that As is mainly associated with sulfur in nails and hair. Nails, rather than hair and urine, could be used as a proper biomarker for arsenicosis. High ADD from the environment and low excretion could result in As toxicity to humans.
Environmental Science & Technology 04/2013; · 4.80 Impact Factor
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ABSTRACT: Hydroxylated polybrominated diphenyl ethers (OH-PBDEs), methoxylated PBDEs (MeO-PBDEs) and PBDEs were determined in three mollusk species collected from three Chinese coastal regions in 2007, 2009, 2010 and 2011. The dominant MeO- and OH-PBDEs isomers detected in mollusks were 6-MeO-BDE-47, 2'-MeO-BDE-68, 6-OH-BDE-47 and 2'-OH-BDE-68. Concentrations of ΣMeO-PBDEs ranged from 9.20 to 2090pgg(-1) dry weight (mean: 450pgg(-1) dry weight). Concentrations of ΣOH-PBDEs ranged from 118 to 2540pgg(-1) dry weight (mean: 534pgg(-1) dry weight). Species differences in accumulation were found for the three mollusk species. Spatial distribution showed that OH- and MeO-PBDEs levels were higher in Weihai than in Tianjin. The temporal trends of OH- and MeO-PBDEs in mollusks were studied during period of 2007 to 2011, rising of ΣOH-PBDEs in Rap from Penglai and Ost from Weihai and declining of ΣMeO-PBDEs in Ost in Penglai were observed. Significant correlations were found between OH- and MeO-PBDEs, but neither between PBDEs and OH-PBDEs, nor between PBDEs and MeO-PBDEs, suggesting that OH- and MeO-PBDEs may have a common source or similar accumulation behavior in mollusks. OH- and MeO-PBDEs were likely not to originate from PBDE precursors.
Chemosphere 04/2013; · 3.21 Impact Factor
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ABSTRACT: The residue levels of 16 US EPA priority polycyclic aromatic hydrocarbons (PAHs) and 16 selected organochlorine pesticides (OCPs) in rice and rice hull collected from a typical e-waste recycling area in southeast China were investigated from 2005 to 2007. PAHs and OCPs also were measured in ten mollusk species (soft tissues) collected in an adjacent bay in 2007. Individual PAHs were frequently found in the entire sample set (including the rice, hull, and mollusk samples) with a detection rate of 73 %. The total concentrations of 16 PAHs (ΣPAHs) and 16 OCPs (ΣOCPs) were in the range of 40.8-432 ng/g dry weight (mean: 171 ng/g) and 2.35-925 ng/g (122 ng/g), respectively, which were comparable or higher than those reported in some polluted areas. Statistical comparisons suggested that the concentrations of contaminants in hull gradually decreased from 2005 to 2007 and the residue levels were generally in the order of mollusk, hull, and rice, on a dry weight basis. Principal component analysis in combination with diagnostic ratios implied that combustion of coal, wood, and plastic wastes that are closely associated with crude e-waste recycling activities is the main source of PAHs. The finding of decreasing trend of concentrations of PAHs in this area is consistent with the efforts of local authorities to strengthen regulations on illegal e-waste recycling activities. Composition analysis suggested that there is a recent usage or discharge of hexachlorocyclohexane and dichlorodiphenyltrichloroethane into the tested area. The estimated daily intake (EDI) of ΣPAHs and ΣOCPs (calculated from mean concentrations) through rice and mollusk consumption was 0.411 and 0.921 μg/kg body weight (bw)/day, respectively.
Environmental Geochemistry and Health 04/2013; · 1.62 Impact Factor
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ABSTRACT: A novel method for selective determination of Cr(III) and Cr(VI) in environmental water samples was developed based on target-induced fluorescence quenching of glutathione-stabilized gold nanoclusters (GSH-Au NCs). Fluorescent GSH-Au NCs were synthesized by a one-step approach employing GSH as reducing/protecting reagent. It was found that Cr(III) and Cr(VI) showed pH-dependent fluorescence quenching capabilities for GSH-Au NCs, and thus selective determination of Cr(III) and Cr(VI) could be achieved at different pHs. Addition of EDTA was able to effectively eliminate the interferences from other metal ions, leading to a good selectivity for this method. Under optimized conditions, Cr(III) showed a linear range of 25-3800μgL(-1) and a limit of detection (LOD) of 2.5μgL(-1). The Cr(VI) ion demonstrated a linear range of 5-500μgL(-1) and LOD of 0.5μgL(-1). The run-to-run relative standard deviations (n=5) for Cr(III) and Cr(VI) were 3.9% and 2.8%, respectively. The recoveries of Cr(III) and Cr(VI) in environmental water samples were also satisfactory (76.3-116%). This method, with its simplicity, low cost, high selectivity and sensitivity, could be used as a promising tool for chromium analysis in environmental water samples.
Analytica chimica acta 04/2013; 770:140-6. · 4.31 Impact Factor
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ABSTRACT: Metal detector: The title strategy provides a new way for rapid profiling of the metal-associated proteins on a proteome- and metallome-wide scale. The technique was applied to identify protein targets of a bismuth-based drug in Helicobacter pylori and to study the metal binding of the protein SlyD, which is a member of the FK506-binding protein family, in E. coli.
Angewandte Chemie International Edition 04/2013; · 13.45 Impact Factor
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ABSTRACT: An extraction procedure for extracting organic mercury species including methylmercury (MeHg) and ethylmercury (EtHg) from petroleum samples was developed. Three extraction methods (shaking, ultrasonic and microwave assisted extraction) using different extraction solvents (TMAH, KOH/CH3OH, HCl and acidic CuSO4/KBr) were investigated by comparing the extraction efficiency of the organic mercury species. Microwave assisted extraction at 60W for 5min using TMAH (tetramethylammonium hydroxide, 25%, m/v) provided the most satisfactory extraction efficiency for MeHg and EtHg in petroleum at 86.7%±3.4% and 70.6%±5.9%, respectively. Speciation analysis of mercury was done by on-line coupling of high performance liquid chromatography with cold vapor generation atomic fluorescence spectrometry (HPLC-CV-AFS). The proposed method was successfully applied to analyze several crude oil and light oil samples. The concentrations of MeHg ranged from under detection limit to 0.515ngg(-1), whereas EtHg was not detected in the samples. This method can be a very useful tool in evaluating the risk of mercury emissions from petroleum.
Talanta 03/2013; 106C:60-65. · 3.79 Impact Factor
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ABSTRACT: To be mild! Mild oxidization of chemically converted graphene with diluted nitric acid produces low-oxidation and low-defect acid-oxidized graphene (AOG) material with excellent water dispersibility. In MALDI MS, the AOG matrix yielded significantly higher signals than graphene, graphene oxide, and conventional organic matrices for nonpolar analytes.
Chemistry 03/2013; · 5.93 Impact Factor
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ABSTRACT: Polyvinyl pyrrolidone polymer (PVP) has been widely applied in biological and medical fields. A few in vitro studies indicated that PVP might cause toxicity. However, the underlying mechanism is poorly understood. In this work, we found that PVP directly induced strand breakages of various DNA molecules, implicating a cleavage activity. Moreover, reactive oxygen species (ROS) scavenging analysis shows that DNA cleavage activity of PVP is not related to ROS-induced oxidation. As revealed by gel electrophoresis and liquid chromatography/mass spectrometry analysis, the major cleavage products of DNA were identified as two purine bases, guanine and adenine, suggesting that PVPs have a novel depurination activity. The selective depurination and DNA cleavage activity of PVPs were further confirmed by studying the interaction of PVP with four nucleosides and four well-designed oligodeoxynucleotides probes containing specific nucleotides. This study may provide insights into PVP-DNA interactions and resultant genotoxicity and may also open a new way for DNA study.
Environmental Science & Technology 03/2013; · 4.80 Impact Factor
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Nuoya Yin,
Qian Liu,
Jiyan Liu,
Bin He,
Lin Cui,
Zhuona Li,
Zhaojun Yun,
Guangbo Qu,
Sijin Liu,
Qunfang Zhou, Guibin Jiang
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ABSTRACT: The impact of silver nanoparticles (AgNPs) on the central nervous system is a topic with mounting interest and concern and the facts remain elusive. In the current study, the neurotoxicity of commercial AgNPs to rat cerebellum granule cells (CGCs) and the corresponding molecular mechanism are closely investigated. It is demonstrated that AgNPs induce significant cellular toxicity to CGCs in a dose-dependent manner without damaging the cell membrane. Flow cytometry analysis with the Annexin V/propidium iodide (PI) staining indicates that the apoptotic proportion of CGCs upon treatment with AgNPs is greatly increased compared to the negative control. Moreover, the activity of caspase-3 is largely elevated in AgNP-treated cells compared to the negative control. AgNPs are demonstrated to induce oxidative stress, reflected by the massive generation of reactive oxygen species (ROS), the depletion of antioxidant glutathione (GSH), and the increase of intracellular calcium. Histological examination suggests that AgNPs provoke destruction of the cerebellum granular layer in rats with concomitant activation of caspase-3, in parallel to the neurotoxicity of AgNPs observed in vitro. Taken together, it is demonstrated for the first time that AgNPs substantially impair the survival of primary neuronal cells through apoptosis coupled to oxidative stress, depending on the caspase activation-mediated signaling.
Small 02/2013; · 8.35 Impact Factor
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ABSTRACT: A total of 60 paired samples of earthworm, corresponding soil and wormcast were collected to investigate the bioaccumulation tendency of polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in earthworms from a typical E-waste dismantling area in east China. Significant correlations were observed for the total concentrations among different matrix types except for PCDD/Fs in soil and earthworm. The bioaccumulation tendency showed some differences among the contaminants. Calculated biota-soil accumulation factors (BSAFs) indicated that PCBs and PBDEs had higher bioaccumulation potential compared to PCDD/Fs, which was somewhat different from laboratory studies. The plot of mean BSAFs versus log K(ow) values for PCBs and PBDEs was well fitted by a second-order polynomial with the maximum BSAF at approximately log K(ow) of 6.5. While for PCDD/Fs, only a slightly decreasing trend was observed with increasing log K(ow). Composition analysis indicated that tetra-, penta- and hexa-halogenated homologs had higher bioaccumulation levels, indicating that medium-halogenated congeners with log K(ow) around 6.5 are more easily accumulated by earthworms. Furthermore, the ratios of BDE-47/-99 and BDE-99/-100 showed some discrepancies with the technical products and other biotic species, suggesting different bioaccumulation potential of PBDEs in earthworm.
Environment international 02/2013; 54C:50-58. · 4.79 Impact Factor
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ABSTRACT: Polybrominated diphenyl ethers (PBDEs) along with hydroxylated polybrominated diphenyl ethers (OH-PBDEs) and methoxylated polybrominated diphenyl ethers (MeO-PBDEs) were found in plant and soil samples collected surrounding a seafood processing factory and a seafood market in China. The profiles of MeO-PBDE congeners were different between seafood processing factory and seafood market. The detection frequency and concentration of 6-OH-BDE-47 were lower than that of MeO-PBDEs. Near seafood processing factory, a decreasing trend of analyte concentrations in plants was found downstream the river where factory wastewater was discharged. Concentrations of ΣMeO-PBDEs in plant and soil samples showed difference as root > soil > leaf. However, at seafood market, the concentrations of ΣMeO-PBDEs were much higher in leaves than those in soil. The concentration of ΣMeO-PBDEs in leaves showed a remarkable difference between Calystegia soldanella (Linn.) R. Br. and Setaira viridis (L.) Beauv.
Environmental pollution (Barking, Essex: 1987) 02/2013; 176C:100-105. · 3.43 Impact Factor
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ABSTRACT: The concentrations and geographical distribution of hexabromocyclododecane (HBCD) were investigated in 37 composite surface sediments from seven major river drainage basins in China, including Yangtze River, Yellow River, Pearl River, Liaohe River, Haihe River, Tarim River and Ertix River. The detection frequency of HBCD was 54%, with the concentrations ranged from below limit of detection (LOD) to 206 ng/g dry weight. In general, the geographical distribution showed increasing trends from the upper reaches to the lower reaches of the rivers and from North China to Southeast China. Compared to other regions in the world, the average concentration of HBCD in sediments from Yangtze River drainage basin was at relatively high level, whereas those from other six river drainage basins were at lower or similar level. The highest HBCD concentration in sediment from Yangtze River Delta and the highest detection frequency of HBCD in Pearl River drainage basins suggested that the industrial and urban activities could evidently affect the HBCD distribution. HBCD diastereoisomer profiles showed that gamma-HBCD dominated in most of the sediment samples, followed by alpha- and beta-HBCD, which was consistent with those in the commercial HBCD mixtures. Further risk assessment reflected that the average inventories of HBCD were 18.3, 5.87, 3.92, 2.50, 1.77 ng/cm2 in sediments from Pearl River, Haihe River, Tarim River, Yellow River and Yangtze River, respectively.
Journal of Environmental Sciences 01/2013; 25(1):69-76. · 1.66 Impact Factor
