ISSN 1001–0742 Journal of Environmental Sciences Vol. 24 No. 11 2012

CONTENTS Aquatic environment Occurrence of selected aliphatic amines in source water of major cities in Haifeng Zhang, Shuoyi Ren, Jianwei Yu, Min Yang ················································································· 1885 Selection of magnetic anion exchange resins for the removal of dissolved organic and inorganic matters Qiongjie Wang, Aimin Li, Jinnan Wang, Chengdong Shuang ······································································ 1891 Reductive transformation and detoxification mechanism of 2,4-dinitrochlorobenzene in combined zero valent iron and anaerobic-aerobic process Jinyou Shen, Zongyuan Zhou, Changjin Ou, Xiuyun Sun, Jiansheng Li, Weiqing Han, Lin Zhou, Lianjun Wang··············· 1900 Fractionation of residual Al in natural water treatment from reservoir with poly-aluminum-silicate-chloride (PASiC): Effect of OH/Al, Si/Al molar ratios and initial pH Zhonglian Yang, Baoyu Gao, Yan Wang, Yaqin Zhao, Qinyan Yue································································· 1908 Effect of solid contents on the controlled shear stress rheological properties of different types of sludge Ting Li, Yili Wang, Yujing Dong ····································································································· 1917 Optimizing the operation of the Qingshitan Reservoir in the Lijiang River for multiple human interests and quasi-natural flow maintenance Qiuwen Chen, Duan Chen, Ruiguang Han, Ruonan Li, Jinfeng Ma, Koen Blanckaert ············································ 1923 Zeolite (Na) modified by nano-Fe particles adsorbing phosphate in rainwater runoff Lili Gan, Jiane Zuo, Bangmi Xie, Peng Li, Xia Huang ·············································································· 1929 Contamination by persistent toxic substances in surface sediment of urban rivers in Chaohu City, China Feipeng Li, Haiping Zhang, Xiangzhou Meng, Ling Chen, Daqiang Yin ·························································· 1934 Fatty acids and algal lipids as precursors of chlorination by-products Yan Liang, Yuen Shan Lui, Huachang Hong ························································································· 1942 Atmospheric environment Uptake of isoprene, methacrylic acid and methyl methacrylate into aqueous solutions of sulfuric acid and hydrogen peroxide Ze Liu, Maofa Ge, Weigang Wang···································································································· 1947

Comparison of PM10 concentrations and metal content in three different sites of the Venice Lagoon: An analysis of possible aerosol sources Daniele Contini, Franco Belosi, Andrea Gambaro, Daniela Cesari, Angela Maria Stortini, Maria Chiara Bove ················· 1954 Seasonal trend of ambient PCDD/Fs in Tianjin City, northern China using active sampling strategy Lei Ding, Yingming Li, Pu Wang, Xiaomin Li, Zongshan Zhao, Qinghua Zhang, Ting Tuan, Guibin Jiang ····················· 1966 Ultrafine particle emission characteristics of diesel engine by on-board and test bench measurement Cheng Huang, Diming Lou, Zhiyuan Hu, Piqiang Tan, Di Yao, Wei Hu, Peng Li, Jin Ren, Changhong Chen··················· 1972 N-doped mesoporous alumina for adsorption of carbon dioxide Jayshri A. Thote, Ravikrishna V. Chatti, Kartik S. Iyer, Vivek Kumar, Arti N. Valechha, Nitin K. Labhsetwar, Rajesh B. Biniwale, M. K. N. Yenkie, Sadhana S. Rayalu··········································································· 1979 Terrestrial environment Extraction of heavy metals from e-waste contaminated soils using EDDS Renxiu Yang, Chunling Luo, Gan Zhang, Xiangdong Li, Zhenguo Shen··························································· 1985 Characterization of contamination, source and degradation of petroleum between upland and paddy fields based on geochemical characteristics and phospholipid fatty acids Juan Zhang, Renqing Wang, Xiaoming Du, Fasheng Li, Jiulan Dai ································································ 1995 Environmental biology Bacterial diversity and distribution in the southeast edge of the Tengger Desert and their correlation with soil enzyme activities Wei Zhang, Gaosen Zhang, Guangxiu Liu, Zhibao Dong, Tuo Chen, Manxiao Zhang, Paul J. Dyson, Lizhe An················ 2004 Biodegradation of p-cresol by aerobic granules in sequencing batch reactor Farrukh Basheer, I. H. Farooqi ········································································································ 2012 Environmental health and toxicology Characterisation of acute toxicity, genotoxicity and oxidative stress posed by textile effluent on zebrafish Wenjuan Zhang, Wei Liu, Jing Zhang, Huimin Zhao, Yaobin Zhang, Xie Quan, Yihe Jin ········································ 2019 Characterization of cytotoxicity of airborne particulates from urban areas of Lahore Badar Ghauri, M. Mansha, Christian Khalil ·························································································· 2028 Serial parameter: CN 11-2629/X*1989*m*150*en*P*20*2012-11

jesc.ac.cn Available online at www.sciencedirect.com JOURNAL OF ENVIRONMENTAL SCIENCES ISSN 1001-0742 CN 11-2629/X Journal of Environmental Sciences 2012, 24(11) 1934–1941 www.jesc.ac.cn

Contamination by persistent toxic substances in surface sediment of urban rivers in Chaohu City, China

Feipeng Li, Haiping Zhang∗, Xiangzhou Meng, Ling Chen, Daqiang Yin

College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China. E-mail: [email protected]

Received 13 January 2012; revised 21 May 2012; accepted 24 May 2012

Abstract The concentration and spatial distribution of persistent toxic substances (PTS) in the river sediment in Chaohu City, China were investigated. A total of nine surface sediments were collected and the selected PTS pollutants including six heavy metals and nineteen polybrominated diphenyl ethers (PBDEs) were analyzed. The mean heavy metal concentrations (in mg/kg, dry weight) ranged within 0.18–1.53 (Hg), 50.08–200.18 (Cu), 118.70–313.65 (Zn), 50.77–310.85 (Cr), 37.12–92.72 (Pb) and 13.29–197.24 (As), and Cu, Zn and As have been regarded as the main metal pollutants. The levels of PBDEs (1.2–12.1 ng/g) and BDE-209 (2.4–30.5 ng/g) were at the middle level of the global range. BDE-209 was the predominant congener (67.0%–85.7%), which agrees with the fact that technical deca-BDE mixtures are the dominant PBDE formulation in China. The relative high level of PTS pollutants in the western part of the city is probably owing to the intensive agricultural activities and lack of sewerage system there. The ecological risk assessment with the sediment quality guidelines (SOGs) indicates that the urban river sediments in the city have been heavily contaminated by heavy metals with probable ecotoxicological impacts on freshwater organisms and the main toxic pollutants are Hg and As. The results of current study imply that the city, and perhaps many other small cities in China as well, requires immediate pollution control measures with emphasis on not only conventional organic pollutants but also on PTS such as heavy metals and PBDEs. Key words: heavy metal; polybrominated diphenyl ethers; sediment; urban river; Chaohu City DOI: 10.1016/S1001-0742(11)61033-4

Introduction pollutants in aquatic system, sediment may give rise to secondary pollution events via the geochemical circulation Urban river systems are subject to rapid changes in physi- of toxic pollutants and pose serious ecological risks in cal, hydrological and chemical conditions owing to various surrounding areas (Lohani et al., 2008; Reza and Singh, human disturbances. These rivers are usually managed as 2010; Ma et al., 2010). The level of contamination in the resources for human living benefits such as water land- sediment is closely linked to the health of the ecosystem scape, flood mitigation and water supply. Unfortunately, as a whole (Pekey, 2006). Therefore there is a demand the river pollution has become one of the most serious of more concern on sediment health of urban rivers for problems of urban environment owing to the increasing maintaining ecological quality. influxes of nutrients, metals and other chemicals with Many previous studies have widely confirmed the se- dispersed loadings (Taylor et al., 2009). Many studies rious contamination of river sediment by heavy metals have confirmed that human activities (e.g. industrial, do- (Aktar et al., 2010; Taghinia et al., 2010; Bing et al., 2011; mestic and transport) are the main reasons that enhance Wang et al., 2011) and POPs (Feng et al., 1998; Minh the concentrations of toxic contaminants including heavy et al., 2007; Ying et al., 2009) in urban areas. In China, metals and persistent organic pollutants (POPs) in urban heavy metal contamination is one of the key government rivers, and cause significant degradation of the related concerns and five elements (Hg, Cr, Cd, Pb and As) environments (Parolini et al., 2010; Singh et al., 2005). have been included in the target of Total Load Control These toxic pollutants existing in water and air, after in the 12th Five-Year Plan of Environmental Protection. their incorporation in sediments through adsorption and Although a number of surveys have been conducted of deposition processes, may be released back into water heavy metal contamination in sediments for large rivers column and atmosphere as a result of the variations of like River (Li et al., 2000; Feng et al., 2004; Wang water physicochemical parameters and biological activity et al., 2011), (Li et al., 2010) and estuarine (de Miguel et al., 2005). As both source and sink of areas (Ip et al., 2007), information regarding the heavy metal concentration in urban river sediments is limited * Corresponding author. E-mail: [email protected] jesc.ac.cn No. 11 Contamination by persistent toxic substances in surface sediment of urban rivers in Chaohu City, China 1935

(Zheng et al., 2008). In a large number of studies on POPs in sediments (Yang et al., 2009, 2011; Chi, 2009; Jiang et al., 2007), the main organic pollutants were polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs). Up to now, studies on the new type of POPs, polybrominated diphenyl ethers (PBDEs) pollution in the sediment of urban rivers are very limited (Chen et al., 2009). Located in middle Anhui Province, East China, Chaohu City has been undergoing rapid development since mid- 1990s. The city has a long history of the production of cements, petrochemicals, nonferrous metal smelting and plastic materials. Similar to the situation in many devel- oping countries, however, environmental protection often River Landscape Residential area gives way to economic development and industrialization Shopping centre in China, in particular in small cities. As one of the Industrial area third-tier cities of China, Chaohu City constructed its first Fig. 1 Map of Chaohu City and sampling sites (CH1–CH9). municipal wastewater treatment plant in 2001 with the 1.2 Sample collection and analysis capacity of 60,000 m3/day, serving the central downtown area only and leaving the rest of the city without any The sampling locations have been selected to reflect the sewage collection and delivery system. Urban rivers in the pollution features of the city with various types of ex- city have been overburdened with sewage demands and posure, including landscape, agricultural land, shopping maintenance of their quality relies heavily on flushing by center and residential area (Fig. 1). Nine surface sediment the neighboring Chaohu Lake. Until now there have been samples were collected from the rivers in July 2010 using a no regular water quality monitoring programs for the rivers stainless steel grab sampler. Immediately after collection, of the city. the samples were wrapped in two layers of aluminum foil, The aim of this study is to comprehensively investigate sealed in plastic bags and stored in a cool box with ice. the concentration and spatial distribution of the PTS in Upon arrival in the laboratory, the samples were freeze- the sediment of urban rivers of Chaohu City. Furthermore, dried, mixed thoroughly, sieved to 100 mesh and kept at the ecological risk was also assessed. Such investigation –18°C for analysis. will provide the pollution information in the area, help Metal concentrations were determined by total sedi- understanding the urban pollution situations particularly in ment digestion following standard procedures of US EPA small cities of China, and provide implications of future Method 3052. The digestion process was carried out by pollution control strategies for these cities. the microwave digestion apparatus (ETHOS 1, Milestone Srl, Italy) with automatic pressure and temperature regu- 1 Materials and methods lation. Dried sample of 0.25 g was put into pre-cleaned polytetrafluoroethene vessels with 12 mL HNO3-HF (3:1, 1.1 Study area V/V) acid mixture solutions in a fume hood. Thereafter, the ◦ ′ ◦ ′ vessels were sealed and heated in the microwave system Chaohu City (31 36 N, 117 51 E) is located in Anhui with the typical reaction temperature profile (digest at Province, near Chaohu Lake (Fig. 1) with an area of 2080 2 180°C for 15 min, rise to 200°C in 14 min and remain km and an urban population of 1.0 million in 2010. There at 200°C for 9 min). When the microwave program was are in total six rivers (Tian, Yuxi, Lujia, East Huancheng, finished, samples were removed from microwave system Dinggang and West Huancheng) and an artificial lake Xier and cooled near room temperature; 3 drops of HClO4 were Pond in the city, most of which are narrow and shallow due added into the vessels and heated at 150°C for 50 min. to severe sedimentation. Details of each river are shown in After digestion and cooling, samples were filtered and the Table 1 from a field investigation in January 2010. Two filtrate was diluted to 25 mL with 4% HNO3. rivers, Tian and Yuxi, flow through the city and connect Seven heavy metals of great environmental significance the Chaohu Lake to the Yangtze River. have been chosen for analysis in the investigation, in- cluding five elements (Hg, Cr, Cd, Pb and As) in the Table 1 Information of urban rivers of Chaohu City target of Total Load Control in the 12th Five-Year Plan of River Length Width (m) Depth (m) Surface Environmental Protection and other two elements (Cu and (m) area (km2) Zn) which have been frequently detected as main metal pollutants in urban rivers of China. The metal ions (Cu, Tian 3000 120–150 0.9–7.1 0.13 Yuxi 57400 125–145 4.2–5.0 3808 Zn, Cr, Cd, Pb and As) were measured by Inductively Lujia 2068 20–43 0.5–2.9 0.06 Coupled Plasma Atomic Emission Spectrometer (ICP- East Huancheng 1673 13–36.5 0.5–2.4 0.08 AES, Optima 2100 DV, PerkinElmer Inc., USA). The Dinggang 685 32–60 0.6–0.8 0.03 West Huancheng 2483 16–70 0.5–2.2 0.12 concentrations of Hg were analyzed by Direct Mercury Analyzer (DMA80, Milestone Srl, Italy) using directly dry

jesc.ac.cn 1936 Journal of Environmental Sciences 2012, 24(11) 1934–1941 / Feipeng Li et al. Vol. 24 soil samples without digestion process. For quality control, min), and 290°C at 5°C/min (held for 15 min). For BDE- reagent blanks, replicates and standard reference materials 196, 206 and 209, a DB-5 (15 m×0.25 mm i.d., 0.1 µm (GBW 07403 (GSS-3)), purchased from National Research film thickness) capillary column (J&W Scientific, Folsom, Center for Geoanalysis (China), representing 10%, 20% USA) was employed. The oven temperature was initiated and 10% of the total sample population, respectively, were at 110°C (held for 5 min) and increased to 200°C at a incorporated in the analysis to detect contamination and rate of 20°C/min (held for 4.5 min) and 310°C at a rate to assess accuracy and bias. The analytical results showed of 10°C/min (held for 20 min). Ultrahigh purity helium no signs of contamination and that the precision and bias was used as the carrier gas. The transfer line, ion source of the analysis were lower than 10%. The recovery rates and quadrupole temperatures were maintained at 280, 250 for all of the heavy metals were around 80% to 95%. The and 300°C, respectively. Quantification of PBDEs was detection limits for metals are lower than 10 µg/L. Cd has performed using an external standard method. The limit been excluded from discussion in this article owing to its of detection (LOD) is 50 pg/g for BDE-209 and 3 pg/g for very low levels in the sediment samples. other congeners based on dry weight. Forty two PBDE congeners as targets were purchased For each batch of nine sediment samples, a procedural from AccuStandards (New Haven, CT, USA), including blank, a spiked blank, a matrix spiking sample (forty two three mono-BDEs (BDE-1, 2, and 3), seven di-BDEs PBDE congeners spiked into sample) and a matrix spiking (BDE-7, 8, 10, 11, 12, 13, and 15), eight tri-BDEs (BDE- duplicate were processed. The recoveries of forty two 17, 25, 28, 30, 32, 33, 35, and 37), six tetra-BDEs PBDE congeners, BDE-50 and BDE-172 were 83.2% ± (BDE-47, 49, 66, 71, 75, and 77), seven penta-BDEs 18.4%, 66.2% ± 13.9% and 80.8% ± 11.8%, respectively. (BDE-85, 99, 100, 116, 118, 119, and 126), five hexa- Low level of BDE-209 (about the LOD) was found in BDEs (BDE-138, 153, 154, 155, and 166), four hepta-BDE procedural blanks and subtracted from the sample mea- (BDE-181, 183, 190, and 196), nona-BDE (BDE-206) and surement. deca-BDE (BDE-209). BDE-50 and BDE-172 as surrogate Total organic carbon (TOC) was analyzed with the standards were also purchased from AccuStandards. Shimadzu TOC-VCPN with solid sample module (SSM- Detailed analytical procedure and instrumental analysis 5000A, Japan). The overall standard deviation of measure- conditions are given elsewhere (Mai et al., 2005). About ments is lower than 3% (n = 3). 3.0 g sediment samples were spiked with BDE-50 and 1.3 Statistical analysis BDE-172 and Soxhlet extracted with a mixture of acetone and hexane (1:1, V/V) for 48 hr. Activated copper were Statistical analysis of the data was performed by SPSS added into samples prior to extraction to remove elemental v.13.0. Pearson multiple correlation analysis was applied sulfur. The extract was concentrated and purified further on to the results between toxic pollutants and TOC at 0.01 a glass column packed with 3% water deactivated silica gel and 0.05 levels. and basic alumina. Target PBDEs were eluted in the 50 mL fraction of 50% DCM in hexane (V/V), and the final extract 2 Results and discussion volume was reduced to 200 µL under a gentle N2 stream. Extracts were analyzed with a Shimadzu Model 2010 GC- 2.1 Levels and spatial distribution MS (Japan) using negative chemical ionization in selected ion monitoring mode. A DB-5 (30 m×0.25 mm i.d., 0.25 The levels of six heavy metals at nine sampling sites are µm film thickness) capillary column (J&W Scientific, shown in Table 2. The concentrations of heavy metals / Folsom, USA) was used for the determination of PBDE (in mg kg dry weight (dw)) range within 0.18–1.53 (Hg), congeners except for BDE-196, 206 and 209. The column 50.08–200.18 (Cu), 118.70–313.65 (Zn), 50.77–310.85 temperature was initiated at 110°C (held for 1 min) and (Cr), 37.12–92.72 (Pb) and 13.29–197.24 (As). The heavy increased to 180°C at 8°C/min (held for 1 min), 240°C at metal concentrations observed in Chaohu City are general 2°C/min (held for 5 min), 280°C at 2°C/min (held for 25 higher than in other large cities in China (Table 3). The concentrations of Hg and As are about 3 times higher than

Table 2 Measured heavy metal concentrations and background values (unit: mg/kg dw)

Site River Hg Cu Zn Cr Pb As

CH1 Tian 0.20 52.86 121.12 71.08 54.77 197.24 CH2 Tian 0.18 50.08 118.70 50.77 41.25 13.29 CH3 Yuxi 0.27 70.63 185.09 80.36 37.12 27.59 CH4 Xier Pond 0.22 61.85 195.90 94.13 39.12 32.08 CH5 Lujia 0.35 61.72 207.68 84.43 40.32 31.01 CH6 Dinggang 0.74 77.78 265.08 75.88 50.72 24.16 CH7 West Huancheng 0.68 79.21 313.65 70.43 49.08 24.84 CH8 West Huancheng 1.53 200.18 290.00 310.85 92.72 23.56 CH9 East Huancheng 0.26 60.65 157.43 80.36 40.03 25.42 B 0.20 20.20 56.30 67.00 26.00 – TEL 0.17 36.00 123.00 42.00 35.00 7.20 PEL 0.49 197.00 315.00 160.00 91.00 42.00 B: background values from Shi et al., 2010; TEL: threshold effect level; PEL: probable effect level.

jesc.ac.cn No. 11 Contamination by persistent toxic substances in surface sediment of urban rivers in Chaohu City, China 1937

Table 3 Comparison of mean heavy metal concentrations in surface sediments of urban rivers (unit: mg/kg dw)

Region Hg Cu Zn Cr Pb As Reference

Yangtze River at Wuhan Section 0.26 60.03 230.39 108.00 49.19 15.44 Wang et al., 2011 at Lanzhou Section – 18.49 78.53 – 16.13 – Wang et al., 2010 Pearl River at Guangzhou Section – 348.00 383.40 93.10 102.60 – Niu et al., 2009 of Shanghai 0.13 55.90 114.00 55.60 22.60 – He, 2009 Second of City – 23.58 90.29 49.42 23.76 – Lin et al., 2008 Nanfei River of Hefei City 0.23 32.33 365.95 69.74 50.83 – Shi et al., 2010 Chaohu Lake 0.08 26.18 102.08 60.20 20.70 – Shi et al., 2010 Rivers of Chaohu City 0.49 79.44 206.07 102.03 49.46 44.35 Present study in Yangtze River at Wuhan Section. Compared with other rivers of downtown area have received higher inputs of waters in this region (Nanfei River and Chaohu Lake), anthropogenic trace metal. CH3 is located at the Yuxi River rivers of Chaohu City are obviously suffering from much which receives the water released from the downtown heavier metal pollution. rivers and has shown an elevated level of pollution in the As shown in Table 2, there is significant difference sediment than CH1 and CH2. in concentrations among sampling sites for each type of Nineteen PBDE congeners have been detected in all nine heavy metals. The highest Hg, Cu, Cr and Pb values were surface∑ sediment samples. Table 4 presents a summary of observed at station CH8 while the maximum concentration the PBDEs concentrations (BDE-209 is excluded) and of Zn was found at station CH7 in the West Huancheng BDE-209∑ concentrations in the samples. The concentration River. The extremely high concentration of As was ob- of PBDEs varies from 1204.06 to 12113.14 pg/g with a / served at sampling site CH1 near Chaohu Gate, where mean value of 4995.89 pg g. Compared∑ with the reported it was found to be about 10 times higher than in other levels in literature (Table 5), the PBDEs and BDE-209 sites, the reason of which is currently unknown and is concentrations in Chaohu City are at the middle level of subject to further investigation. In general, the heavy metal the global range, a bit higher than in Yangtze River (Chen levels in the western part of the city are higher than in et al., 2006) and Daliao River (Zhao et al., 2011), and much the eastern part. It agrees with the fact that there are lower than in Pearl River and its tributary Dongjiang River, still many agricultural activities (e.g., vegetable growth South China (Mai et al., 2005). The generally low PBDE and livestock-raising) and lack of sewerage system in the level found in present study is presumably due to the small western part, while it is more like a commercial city with quantity of PBDE flame retardants, especially the technical complete sewerage system in the eastern part. Sites CH1– penta-BDEs products, used in the region. CH3 reflect the pollution level of the two rivers Tian and ∑ As shown in Table 4, the highest concentrations of Yuxi, which are located at the southern fringe of the city PBDEs (12113.14 ng/g) and BDE-209 (72537.85 pg/g) and are out of the downtown. Except for the extremely high were observed in the sampling site CH7 in the middle As concentration in CH1 and average Pb concentrations ∑West Huancheng River. Relatively high concentrations of in CH1 and CH2 compared with other sites, less heavy PBDEs and BDE-209 also occurred in West Huancheng metal contamination has been found in two sites CH1 River (CH6 and CH8) and West Tian River (CH2), which and CH2 in general, indicating that the sediments in the is located in the western part of Chaohu City.

Table 4 PBDEs concentrations in surface sediments (unit: pg/g)

CH1 CH2 CH3 CH4 CH5 CH6 CH7 CH8 CH9

BDE-17 20.26 21.28 12.50 23.54 11.55 4.00 4.99 7.02 12.16 BDE-33 3.27 1.20 4.43 2.47 1.21 0.97 2.35 1.79 1.77 BDE-28 96.75 88.61 61.56 120.10 47.45 21.44 30.26 44.69 36.98 BDE-49 61.51 103.56 46.22 57.33 56.12 57.21 66.74 369.74 58.98 BDE-47 106.53 142.69 73.46 126.73 39.02 64.32 93.70 240.64 73.92 BDE-66 33.17 61.95 22.89 78.88 9.88 19.55 21.96 64.30 28.45 BDE-100 21.30 33.00 70.73 28.88 4.72 25.85 41.29 76.83 18.88 BDE-99 146.69 237.68 86.98 289.03 18.79 56.30 69.09 179.97 56.17 BDE-154 38.13 65.61 25.48 30.68 14.90 46.08 89.97 74.10 24.52 BDE-153 77.76 252.93 111.90 30.28 17.42 161.28 163.51 261.40 73.17 BDE-138 9.32 29.77 10.44 4.95 2.98 15.25 17.55 16.63 0.31 BDE-183 109.82 340.67 131.27 70.25 51.84 155.43 222.67 285.52 102.67 BDE-190 10.81 109.09 23.14 46.99 13.43 31.23 60.74 21.89 13.04 BDE-196 138.93 296.21 203.19 88.29 74.16 366.66 767.54 355.59 206.76 BDE-203 263.70 522.10 290.08 116.46 105.46 776.48 838.29 557.75 236.83 BDE-208 270.50 756.96 538.56 211.60 168.43 1031.47 1770.04 844.71 693.98 BDE-207 472.59 1440.08 957.82 352.86 271.66 1654.33 3156.82 1460.31 1091.61 BDE-206∑ 610.30 1795.95 770.14 448.79 295.04 2233.19 4695.63 1769.53 1202.57 PBDEs 2491.34 6299.34 3440.79 2128.11 1204.06 6721.04 12113.14 6632.41 3932.77 BDE-209 6927.18 26223.20 8530.37 6749.70 2444.48 30535.00 72537.85 17927.12 12365.54

jesc.ac.cn 1938 Journal of Environmental Sciences 2012, 24(11) 1934–1941 / Feipeng Li et al. Vol. 24

Table 5 Comparison of PBDEs levels in surface sediments (ng/g dw) ∑ Region Congeners* PBDEs* BDE-209 Reference

Urban rivers of Chaohu City 18 1.20–12.11 (4.99) 2.44–72.54 (20.47) Present study Niagara River, North America 9 0.72–148.00 – Samara et al., 2006 Cinca River, Spain 6 0.30–34.10 2.10–39.90 Eljarrat et al., 2004 Yangtze River, China 12 0–0.55 (0.15) 0.16–94.6 (13.4) Chen et al., 2006 Pearl River, China 9 1.10–49.30 (12.90) 26.30–3580 (890) Mai et al., 2005 Dongjiang River, China 9 2.20–94.70 (20.70) 21.30–7341 (1440) Mai et al., 2005 Xijiang River, China 9 0.13–0.59 (0.36) 1.95–77.41 (16.06) Mai et al., 2005 Beijiang River, China 9 0.019–0.91 (0.20) 0.23–103.50 (11.66) Chen et al., 2009 Daliao River, China 26 0.017–0.20 (0.070) 0.11–1.85 (0.58) Zhao et al., 2011 Fuhe River, China 13 11.80–292.70 (102.60) Hu et al., 2010 * BDE-209 excluded; values in parentheses are average concentrations.

2.2 Relationship between PTS and TOC a relative number calculated by dividing the measured content of a metal by its background value, may directly Organic matter content in sediment is an important fac- reveal the environmental quality and can be used as an tor controlling the sorption of trace metals and organic index of evaluating the geochemical imbalance owing to compounds (Rubio et al., 2000). TOC values in the nine elevated trace metal concentrations which normally are samples varied from 3.12% to 8.05%, with the average attributed to anthropogenic activities (Birch and Taylor, value of 5.20%. Table 6 presents correlation coefficients 1999). The background values of Chaohu Lake are listed for heavy metals and TOC levels in the surface sediments, in Table 2 (not available for As). Figure 2 shows the heavy indicating that TOC is significantly correlated with Hg, Cu, metal contamination index PI for the sediment samples. Cr and Pb. The result shows that TOC plays an important The contamination order of the five metals is Cu > Zn role in the distribution of Hg, Cu, Cr and Pb in the > Hg > Pb > Cr according to the mean PI value of sediments of these urban rivers, but it is not the case for the each metal. The sediment samples have been severely remaining metals. Due to their hydrophobicity, PBDEs are contaminated by Cu and Zn with their PI exceeding 2 for likely to be associated with organic carbon rich in particles. all sampling sites. The statistical analysis of inter-metallic However, there are no significant correlations between relationship showed a high degree of correlation among the PBDE congeners and TOC content. A low correlation ∑ metals (Table 6), implying the identical behavior of metals has been found between TOC and PBDEs (r = 0.22) during its transport in the river environment, though little and BDE-209 (r = –0.132). Poor correlations between correlation of As with other metals has been observed. the PBDEs concentrations and TOC were also reported The distribution pattern of PBDE congeners in surface in sediments of the South China Sea (Mai et al., 2005), Yangtze River (Chen et al., 2006) and Beijiang River (Chen 10 et al., 2009). This may be attributed to the combined Hg Cr 9 effect of transport, mixing and depositional mechanisms Cu Pb associated with PBDEs, though occasional inputs of fresh 8 Zn PBDEs may be another possible reason (Mai et al., 2005). 7 2.3 PTS pollution status and potential sources 6 There are no significant sources that directly discharge 5 pollutants to the rivers of Chaohu City according to the 4 field survey in 2009 and 2010. The PTS pollutants may index Pollution 3 originate from atmospheric deposition or domestic sewage. 2 To assess the pollution status and potential sources of each 1 PTS, a pollution index PI for each type of heavy metals 0 has been applied and the congener distribution pattern of CH1 CH2 CH3 CH4 CH5 CH6 CH7 CH8 CH9 PBDEs analyzed. Site The heavy metal contamination index PI, defined as Fig. 2 Pollution index of heavy metals in surface sediments.

Table 6 Correlation coefficient matrix for trace metals and TOC in surface sediments

Elements Hg Cu Zn Cr Pb As TOC

Hg 1 0.951a 0.772b 0.874a 0.904a –0.256 0.668a Cu 1 0.614 0.975a 0.926a –0.219 0.730a Zn 1 0.475 0.484 –0.428 0.296 Cr 1 0.910 –0.143 0.751a Pb 1 0.098 0.835b As 1 0.440 TOC 1 a Correlation is significant at the 0.05 level; b correlation is significant at the 0.01 level.

jesc.ac.cn No. 11 Contamination by persistent toxic substances in surface sediment of urban rivers in Chaohu City, China 1939

expected below this level, while PEL is often used as the 80 criterion for the prediction of toxicity and corresponds to a ff 70 level above which adverse e ects are frequently expected. Many studies have reported SQGs for heavy metals. In the present study the TEL and PEL values used for Yangtze River have been applied (Wang et al., 2011), which are 8 summarized in Table 2. 7 As shown in Table 2, the concentrations of Hg, Cu, Cr, Pb and As exceed the TEL value for all sediment samples. 6 The element Zn levels are above the TEL value for most 5 sampling locations. The mean concentration of Hg is close 4 to PEL and As is above PEL. The sediments near sampling site CH8 are identified as comprehensively toxic with 3 Relative abundances of PBDE (%) abundances Relative Hg, Cu, Cr and Pb. In general, rivers in Chaohu City 2 can be considered as heavily contaminated with probable ecotoxicological impacts on freshwater organisms. 1 PBDEs are not included in SQGs and the TEL and PEL 0 values are not available in literature. The concentration levels of PBDEs in the sediments may be considered as moderate when compared with aforementioned other BDE-17 BDE-33 BDE-28 BDE-49 BDE-47 BDE-66 BDE-99 BDE-100 BDE-154 BDE-153 BDE-138 BDE-183 BDE-190 BDE-196 BDE-203 BDE-208 BDE-207 BDE-206 BDE-209 studies. Fig. 3 Distribution pattern of PBDE congeners in surface sediments. sediments is shown in Fig. 3. The contribution of BDE- 3 Conclusions 209 to the total PBDEs ranged from 67.0% to 85.7%, with the average value of 76.1%, indicating that deca-BDE for- The pollution levels of selected PTS including heavy mulation is the predominant commercial PBDE products metals and PBDEs in the surface sediments of urban rivers used in the study area. It agrees with the fact that technical in Chaohu City have been investigated. The results show deca-BDE mixtures are the dominate PBDE formulation that the sediments have been heavily contaminated by in China (Zou et al., 2007). Nona-brominated congeners heavy metals, in particular Cu, Zn and As, while the level (BDE-206, BDE-207 and BDE-208) are the second most of PBDEs are moderate compared with those reported abundant homologue group (15.2%) after deca-BDE by in other regions of the global range. The relative high weight of the total BDE inventory, followed by octa-BDE concentration of PTS pollutants in the western part of (BDE-196 and BDE-203), BDE-99, BDE-183 and BDE- the city is probably owing to the intensive agricultural 47, which contribute on average 3.28%, 0.90%, 0.89% activities (e.g. vegetable growth and livestock-raising) and and 0.71%, respectively. The relative amount of nona-BDE lack of sewerage system there. TOC plays an important observed in the study is much larger than expected from the role in the distribution of Hg, Cr and Pb in sediments, but original technical formulations (Alaee et al., 2003). The not the case for the remaining metals and PBDEs under high proportion of nona-BDE and octa-BDE may result study, according to the correlation analysis. The ecological from the debromination of BDE-209 due to microbial risk assessment with SOGs indicates that the urban river degradation and photodegradation during transport (Mai et sediments in the city have been heavily contaminated by al., 2005; Soderstr¨ om¨ et al., 2004). BDE-47 and BDE-99 heavy metals with probable ecotoxicological impacts on are the main components in penta-BDE mixtures, while freshwater organisms and the main toxic pollutants are BDE-183 is often considered as a marker compound for Hg and As. The results of current study imply that the the commercial octa-mix PBDE formulations (Law et city, and perhaps many small cities in China, requires al., 2006). The low-brominated BDEs have been found immediate pollution control measures with emphasis not higher than the composition of commercial products. The only on conventional organic pollutants but also on PTS debromination of higher brominated PBDE congeners and such as heavy metals and PBDEs. atmospheric deposition might be the important source of Acknowledgments low-brominated BDEs (Mai et al., 2005). The study was financially supported by the National Key 2.4 Ecotoxicological concerns Technology R&D Program in the 12th Five-Year Plan The effects of PTS in sediment on freshwater organisms of China: Research & Development on Suitable Key have been assessed according to the sediment quality Technologies of the Village Environmental Monitoring of guidelines (SQGs) for providing an early warning of China (No. 2012BAJ24B01). We would like to express potential problems (Hill et al., 2000). The threshold effect thanks to Dr. Zengsheng Zhang and other students from level (TEL) and the probable effect level (PEL) have Department of Environment Science, Tongji University, been used to evaluate ecotoxicological effects of individual for their assistance in pollution source survey and field heavy metal in sediment based on species toxicity tests (de water quality survey conducted in the summer of 2009 and Deckere et al., 2011). TEL means that no toxic effect is 2010. jesc.ac.cn 1940 Journal of Environmental Sciences 2012, 24(11) 1934–1941 / Feipeng Li et al. Vol. 24

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