Organochlorine Pesticides in Soil, Water and Sediment Along the Jinjiang River Mainstream to Quanzhou Bay, Southeast China

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Organochlorine Pesticides in Soil, Water and Sediment along the Jinjiang River Mainstream to Quanzhou Bay, Southeast China

ARTICLE in ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · DECEMBER 2012 Impact Factor: 2.48 · DOI: 10.1016/j.ecoenv.2012.11.014 · Source: PubMed

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Ecotoxicology and Environmental Safety

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Organochlorine pesticides in soil, water and sediment along the Jinjiang River mainstream to Quanzhou Bay, southeast China

Dan Yang a,b, Shihua Qi b,c,n, Jiaquan Zhang d, Chenxi Wu e, Xinli Xing b,c a Faculty of Engineering, China University of Geosciences, Wuhan 430074, China b State key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China c School of Environmental Studies, China University of Geosciences, Wuhan 430074, China d School of Environmental Science and Engineering, Hubei Polytechnic University, Huangshi 435003, China e Institute of hydrobiology, Chinese Academy of Sciences, Wuhan 430072, China article info abstract

Article history: Residue levels of organochlorine pesticides (OCPs) in multiple compartments (water, soil and Received 28 August 2012 sediment) along the Jinjiang River mainstream to Quanzhou Bay were monitored to elucidate Received in revised form sources and fate. The concentrations of OCPs in surface soil of the watershed of the Jinjiang River 9 November 2012 (2.4471.97 ng/g for hexachlorocyclohexanes (HCHs) and 11.478.46 ng/g for dichlorodiphenyltri- Accepted 12 November 2012 chloroethanes (DDTs)) and the Quanzhou Bay (1.8172.15 ng/g for HCHs and 9.72714.66 ng/g for Available online 20 December 2012 DDTs) were comparable. The concentrations of HCHs and DDTs in dissolved phase were 55–94% for Keywords: the total HCHs and ten to sixteen percent for the total DDTs in the Jinjiang River. High correlations of Organochlorine pesticides (OCPs) OCPs between suspended particulate matter (SPM) and sediment (po0.01) were found in this study, Jinjiang River which demonstrated that OCPs absorbed onto SPM was the major source in the sediment of Quanzhou Bay Quanzhou Bay. The use of lindane was the major source of HCHs in the study region. Dicofol Dissolved phase Suspended particulate matter pollution was found in water of the Jinjiang River and sediment of Quanzhou Bay. Based on the Sediment sediment quality guidelines, DDTs pose more ecotoxicological risk in environment of the Jinjiang River and Quanzhou Bay. & 2012 Elsevier Inc. All rights reserved.

1. Introduction 2008). Furthermore, OCPs can transport and spread among the different environmental media to form the cross contamination. Organochlorine pesticides (OCPs), well known as typical Soil is considered to be an important storage for OCPs. OCPs could persistent organic pollutants (POPs), have adverse effects on spread into aquatic environment through runoff from non-point humans and ecosystems, according to the Stockholm Conven- soil sources. In the aquatic environment, low dose of OCPs might tion of 2009 (UNEP(United Nations Environment Programme), still cause biologically adverse effects on ecosystems (Crisp et al., 2009). There has been an extensive concern for OCPs due to 1998) and the contamination might even hazard the human their high toxicity, persistence, bioaccumulation and biomagni- beings through aquatic food. SPM is an important medium for ficationintheenvironment(Zhang et al., 2002; Wan et al., OCPs on the transportation in aquatic environment. OCPs may be 2005).ChinaisalargeproducerandconsumerofOCPs.Hexa- removed from the water to adsorb on the SPM due to their high chlorocyclohexanes (HCHs) and dichlorodiphenyltrichlor- affinity for organic matter, and finally accumulated in sediment. oethanes (DDTs), the typical OCPs, were widely used in China On the other hand, OCPs in sediment can transport back to water between 1950s and 1980s due to the low cost and high via resuspension (Liu et al., 2008). insecticidal efficacy. Before their officially banned in 1983, the OCPs were once widely used in the agricultural area in total production of HCHs and DDTs in China was about 4.9 and China, especially in the southeast of China (Wang et al., 0.4 million tons, respectively (Fu et al., 2003). 2005). Quanzhou Bay is located in Fujian Province, southeast OCPs were found widespread in the environmental media, China, receiving the import of the Jinjiang River and the such as soil, water, suspended particulate matter (SPM), sedi- Luoyang River. The Jinjiang River is the third largest river in ment, atmosphere and organisms (Cai et al., 2010; Liu et al., Fujian Province and transport a large number of suspended solids to Quanzhou Bay. As an important aquafarm in China, the

n OCPs contaminations in Quanzhou Bay and its source should Corresponding author. require much more attention. However, not many researches E-mail addresses: [email protected] (D. Yang), [email protected] (S. Qi), [email protected] (J. Zhang), were found to show OCPs concentrations in surface soil [email protected] (C. Wu), [email protected] (X. Xing). of the Jinjiang Watershed (Zhang et al., 2011a), and marine

Fig. 1. Location of sampling points.

environment of Quanzhou Bay (Gong et al., 2007; Su et al., 2.3. Instrumental analysis 2006; Yatawara et al., 2010), respectively, without simulta- neous and multimedia researches. This study was carried out to OCP analysis was conducted on an Agilent 7890 A gas chromatograph equipped measure the concentrations of OCPs in the soil and water along with a Ni electron capture detector (GC–ECD). The capillary column used for the analysis was a DB-5 (30 m, 0.32 mm i.d., 0.25 mm film thickness). Nitrogen was used the Jinjiang River and sediment in Quanzhou Bay to display the as carrier gas at 2.5 mL/min under the constant flow mode. Injector and detector contamination status and distribution of OCPs in Quanzhou Bay temperatures were maintained at 290 and 300 1C, respectively. The temperature and its main source river. program used as follows: The oven temperature began at 100 1C (equilibrium time 1 min), raised to 200 1Cat41C/min, then to 230 1Cat21C/min, and at last reached to 280 1C at a rate of 8 1C/min, held for 15 min. A 2 mL sample was injected into the 2. Materials and methods GC–ECD for analysis. Concentrations of individual target OCPs were quantified according to a six-point internal standard calibration curve. 2.1. Sample collection 2.4. Quality assurance The sampling sites are shown in Fig.1. Total of eighteen surface soil samples (0–20 cm) were collected, including eight was in the watershed of the Jinjiang For every set of 10 samples, a procedural blank and spiked sample consisting of all River (JRW) and the other ten was along the coast of Quanzhou Bay (QBC). Each reagents was run to check interference and cross-contamination. No significant peaks soil sample was mixed of four sub samples collected in the 10 10 m2 plot with a overlapping the OCP standards appeared in the chromatograms of the blanks. The pre-cleaned stainless steel scoop. Five water samples were collected along the method detection limits (MDLs) of OCPs were described as 3:1 signal versus noise mainstreams (lower reach) of the Jinjiang River from near surface (0–20 cm value (S/N). The spiked recoveries of OCPs using 20 ng of composite standards were in depth). Each sample was mixed with both sides of the river water at one transect. the range of 75–105%. The relative standard deviation (RSD) ranged from five percent Immediately after collection, the water samples were transported back to the field to ten percent. station for filtration to get dissolved phase (DP) samples. Suspended particulate matter (SPM) samples were collected by filtering water samples through fluorin ethylene filters (50 mm 0.45 mm, Millipore, USA). Sixteen sediment samples 3. Results and discussion were taken in intertidal mud flats along nearby coastal areas of Quanzhou Bay, while eight surface (0–20 cm) and corresponding subsurface (20–40 cm) layers were sampled respectively. All these samples were collected during August 2011. 3.1. OCPs in surface soil of JRW and QBC The soil, sediment and SPM wrapped with aluminum foil samples were stored in sealed polythene bags, during transportation and freeze dried at 20 1C before Concentrations of OCPs compounds in surface soil of JRW and extraction. Water samples were taken using precleaned glass bottles and kept at 4 1C before extraction. QBC were shown in Table 1. Total concentration of HCHs (sum of a-HCH, b-HCH, g-HCH and d-HCH) in surface soil of JRW was in 7 2.2. Extraction procedure the range of 0.41–6.78 ng/g with the mean value of 2.44 1.97 ng/g and that of QBC was between 0.46 and 7.90 ng/g with Filters, or 10 g of dried soil or sediment samples were spiked with 20 ng of the mean value of 1.8172.15 ng/g. The HCHs concentration in 2,4,5,6-tetrachoro-m-xylene (TCmX) and decachlorobi phenyl (PCB209) as recovery the soil of JRW was a little higher than that in QBC, but they were surrogates and were Soxhlet-extracted with dichloromethane for 24 h. Water almost in the same level. In contrast with other regions, the mean samples (1 L) were spiked with 20 ng of TCmX and PCB209 and extracted three values of HCHs concentration in the soil of JRW and QBC were times with 25 mL dichloromethane each time. Activated copper granules were added to the collection flask to remove elemental sulfur. The extraction of OCPs was comparable to those reported in Tibet (0.18–5.38 ng/g) (Fu et al., concentrated and solvent-exchanged to n-hexane and further reduced to 2–3 mL by 2001) and Shanghai (2.41 ng/g) (Jiang et al., 2009) and lower than rotary evaporation. The alumina/silica (v/v¼1:2) gel column (both deactivated with those in Beijing (median 5.25 ng/g) (Zhu et al. 2005) and Tianjing three percent water) was used to purify the extract and OCPs were eluted with 30 mL (median 7.03 ng/g) (Lv et al., 2010), but higher than James Ross of dichloromethane/hexane (v/v¼2/3). Then the eluate was concentrated to 0.2 mL Island (0.49–1.34 ng/g) (Klańova´ et al., 2008) and Wolong Natural under a gentle nitrogen stream and a known quantity of penta-chloronitrobenzene (PCNB) was added as an internal standard prior to gas chromatography–electron Reserve, China (0.23–0.80 ng/g) (Zheng et al., 2009). In the soil of (GC–ECD) analysis. JRW, d-HCH was dominant in HCHs, with mean value of 0.80 D. Yang et al. / Ecotoxicology and Environmental Safety 89 (2013) 59–65 61

70.70 ng/g, while b-HCH (0.8871.74 ng/g) was dominant for with other regions in the world, the DDTs concentrations QBC. Concentration of g-HCH were the lowest in HCHs both in in the soil of both JRW and QBC were much lower than surface soil of JRW (0.4670.44 ng/g) and QBC (0.2570.16 ng/g), Tasman, New Zealand (30–34,500 ng/g) (Gaw et al. 2006), suggesting the possible same source of g-HCH in the soil of the Bacninh, Vietnam (106.79737.12 ng/g) (Toan et al. 2009) study areas. and Germany (23.7–173 ng/g) (Manz et al., 2001). In terms With regards to DDTs, the concentrations ranged from 1.77 of the distribution of DDTs in the JRW, o,p0-DDT and p,p0-DDE to 25.03 ng/g and 1.53 to 53.26 ng/g for DDTs (sum of o,p0- were dominant with nearly same mean value of 3.4473.10 DDT, p,p0-DDE, p,p0-DDD and p,p0-DDT) in the soil of JRW and and 3.4473.36 ng/g, respectively. But for QBC, the most QBC, respectively. The mean value of DDTs in JRW was dominant p,p0DDTrangedfrom0.64to34.27ng/g,witha 11.3678.46 ng/g, which was a little higher than that of QBC mean value of 5.07778 ng/g. However, the concentrations of (9.72714.66 ng/g). The DDTs concentrations in the soil of JRW p,p0-DDD were lowest of DDTs both in the soil of JRW and QBC were in the same level with Mulan River Watershed (1.3271.47 ng/g) and QBC (1.1471.63). (8.1977.28 ng/g) and Qiulu River Watershed (5.26 72.93 ng/ g),nearbyXinghuaBay(Zhang et al., 2011b). When compared 3.2. OCPs in surface water of the Jinjiang River Table 1 Concentrations of OCPs in surface soil of JRW and QBC (dry weight (ng/g)). Total HCHs’ levels in dissolved phase (DP) varied from 10.92 to 17.28 ng/L with a mean value of 14.0472.15 ng/L (Table 2). These Compound JRW (n¼8) QBC (n¼10) levels are nearly same as the Yangtze River (0.55–28.07 ng/L) Mean7SDa Range Mean7SD Range (Tang et al., 2008) and the Liaohe River (6.19–35.19 ng/L) (Gawlik et al., 2000), higher than the Huihe River (0.47–6.13 ng/L) (Feng a-HCH 0.5370.59 0.12–2.06 0.2770.10 0.14–0.52 et al., 2011), but lower than the Qiantang River (0.74–543.1 ng/L) 7 b 7 b-HCH 0.66 0.70 n.d. –2.20 0.88 1.74 n.d. –5.68 (Zhou et al., 2008). When compared with other rivers over the g-HCH 0.4670.44 0.09–1.57 0.2570.16 n.d. –0.67 d-HCH 0.8070.70 0.20–2.29 0.4270.25 0.20–1.03 world, concentration of HCHs in water from the Jinjiang River was o,p0-DDT 3.4473.10 n.d–9.99 2.2471.88 n.d. –6.82 similar to that of the Nestos River, Greek (n.d.68.00 ng/L) p,p0-DDE 3.4473.36 0.27–10.04 1.2871.86 0.30–6.71 (Golﬁnopoulos et al., 2003) and much lower than the Giomti p,p0-DDD 1.3271.47 0.19–3.96 1.1471.63 0.21–5.45 River, India (0.02–4846.00 ng/L) (Singh et al., 2005) and the Kucuk 0 7 7 p,p -DDT 3.16 3.04 0.38–7.55 5.07 9.78 0.64–34.27 Menderes River, Turkey (187.00–337.00 ng/L) (Turgut, 2003). The HCHs 2.4471.97 0.41–6.78 1.8172.15 0.46–7.90 DDTs 11.3678.46 1.77–25.03 9.72714.66 1.53–53.26 concentrations of total DDTs in DP ranked in the range of 2.56– 4.97 ng/L, with a mean value of 3.5670.89 ng/L (Table 2). In a Arithmetic mean7standard deviations. comparison with those reported for other rivers, concentration of b Not detected. DDTs in water of the Jinjiang River was at relatively low levels as the water from the Pearl River (0.52–9.53 ng/L) (Yang et al., 2004), and much lower than the water from the Yamuna River, India Table 2 (66.17–722.94 ng/L) (Kaushik et al., 2008) and the El-Haram, Giza, Concentration of OCPs in DP and SPM of surface water in the Jinjiang River (ng/L). Egypt (2300–61,000 ng/L) (El-Kabbanya et al., 2000). The mean concentrations of HCHs and DDTs in the SPM Compound DP (n¼5) SPM (n¼5) of the Jinjiang River were 5.3774.76 and 25.9773.66 ng/L, Mean7SDa Range Mean7SD Range respectively. Compared with SPM, the concentration of HCHs in the DP accounted for 55–94% of the total HCHs. The concentra- a-HCH 3.9470.69 3.23–5.21 1.6071.58 0.28–4.63 tion levels are very close with the Yangtze River (85–94%) 7 b 7 b-HCH 1.42 0.83 n.d. –2.51 0.66 0.59 n.d.–1.25 (Jiang et al., 2000) and Pearl River (72–92%) (Luo et al., 2004). g-HCH 3.6971.04 2.95–5.76 1.6671.73 0.30–5.05 d-HCH 5.2870.46 4.73–6.05 1.8571.94 0.04–4.49 The concentration of DDTs in SPM accounted for 84–90% of the o,p0-DDT 1.6270.25 1.36–1.88 16.7173.83 12.92–23.79 total DDTs, which was at relatively high level as the research on p,p0-DDE 0.3970.27 0.10–0.89 1.5170.78 0.97–3.03 the Pearl River Delta, where DDTs in SPM reached about 88% 0 p,p -DDD 0.4770.38 0.21–1.22 0.8770.56 0.35–1.92 and 90% of the total DDTs in the Baiertang and Macao water p,p0-DDT 1.0870.25 0.79–1.45 6.8871.51 4.58–8.75 columns, respectively (Luo et al., 2004). The results suggested HCHs 14.0472.15 10.92–17.28 5.3774.76 0.93–14.24 DDTs 3.5670.89 2.56–4.97 25.9773.66 22.85–32.82 that, the behavior of the HCHs in the water environment could be explained by solubility rather than by adsorption to organic a Arithmetic mean7standard deviations. matter in SPM, whereas the DDTs appeared more adsorbability b Not detected. to SPM.

Fig. 2. The partition coefﬁcient (KP) of OCPs in the surface water along the mainstream of the Jinjiang River. 62 D. Yang et al. / Ecotoxicology and Environmental Safety 89 (2013) 59–65

The SPM/DP distribution coefficient (KP) of OCPs was utilized 3.3. OCPs in sediment of Quanzhou Bay in our study (Fig.2), because the KP valueismorerepresentative of what is happening in the field water rather than KOC or KSC The average concentrations of total HCHs in surface sediment (Luo et al., 2004). The result showed the trend of the KP values (SS) (0–20 cm) and subsurface sediment (SSS) (20–40 cm) were for HCHs and DDTs was different from J1 to J5 (Fig.2). It is 0.9270.43 and 1.3571.28 ng/g, while the concentrations of total interesting to find that following the water of the Jinjiang River DDTs in SS and SSS were 4.7372.17 and 3.2072.16 ng/g, running towards Quanzhou Bay (from J1 to J5), the KP of HCHs respectively (Table 3). The status of OCPs contamination were decreased from J1 to J3 and increased from J3 to J5. The possible found in the same low level in SS and SSS, which were compar- reasons may be the salinity or composition of heterogeneous able with sediment in Bohai Sea, China (0.8 ng/g for HCHs and nature of the SPM (such as different soot fractions and different 1.4 ng/g for DDTs) (Hu et al., 2009), East China Sea (0.76 ng/g for particle sizes, etc.) changed in the water body (Means, 1995; HCHs and 3.05 ng/g for DDTs) (Chen et al., 2006) and South India Zhou et al., 1999). Such environmental condition might give (o0.1–4.8 ng/g for HCHs and o0.1–35 ng/g for DDTs) different influence to the distribution of HCHs and DDTs in DP (Senthilkumar et al., 2001), and much lower than North Bohai and SPM in the water. Sea, China (92.51 ng/g for HCHs and 9.23 ng/g for DDTs) (Hu et al., 2010), coastal areas of Vietnam (n.d.–1.00 ng/g for HCHs and 0.31–274 ng/g for DDTs) (Hong et al., 2008) and the Yesilirmak Table 3 River, Turkey (14–16 ng/g for HCHs and 71 ng/g for DDTs) (Bakan Concentration of OCPs in surface (0–20 cm) and subsurface (20–40 cm) layers of and Ariman, 2004). sediment along nearby coastal areas of Quanzhou Bay (dry weight (ng/g)).

Compound SS (n¼8) SSS (n¼8)

Mean7SDa Range Mean7SD Range 3.4. Potential sources of OCPs

a-HCH 0.2370.06 0.16–0.36 0.4270.28 0.18–1.01 Composition and some special ratios of HCH isomers and DDT 7 b 7 b-HCH 0.10 0.25 n.d. –0.76 0.32 0.75 n.d.–2.28 congeners were usually used for indicating the varied sources of g-HCH 0.2070.11 n.d.–0.43 0.1670.19 n.d.–0.57 d-HCH 0.4070.20 n.d.–0.74 0.4470.50 n.d.–1.43 OCPs in the environment. Technical HCH (60–70% a-HCH, 5–12% o,p0-DDT 2.8571.30 n.d.–4.00 1.7871.48 0.00–4.00 b-HCH, ten to twelve percent g-HCH and 6 to tenpercent d-HCH) p,p0-DDE 0.3370.37 0.11–1.30 0.2770.22 n.d.–0.64 (Willett et al., 1998) was ofﬁcially banned in China in the mid- 0 p,p -DDD 0.3570.47 0.07–1.51 0.3070.31 0.00–0.87 1980s. As a substitute, lindane (499% g-HCH) has been used in p,p0-DDT 1.2070.69 0.00–2.59 0.8470.51 0.00–1.36 agriculture since 1990 (Li et al., 2001). Therefore, the -HCH/ - HCHs 0.9270.43 0.36–1.88 1.3571.28 0.20–4.41 a g DDTs 4.7372.17 0.21–7.83 3.2072.16 0.21–5.49 HCH (a/g) ratio is in the range of 3–7 for technical HCH, whereas low a/g ratio depicts the usage of lindane (Li et al., 1998; Toan a Arithmetic mean7standard deviations. et al. 2009). In the present study, a/g ratios (Fig.3) of the soil in b Not detected. JRW and QBC, DP and SPM of water, SS and SSS of Quanzhou Bay

Fig. 3. Mean concentrations of HCH (a) and DDT (b) (y axis on the left) and compositional ratios (y axis on the right) in the environmental media of the study area. D. Yang et al. / Ecotoxicology and Environmental Safety 89 (2013) 59–65 63 were all less than 3, which confirmed the use of lindane as the (po0.01) in this study. This result stressed the OCPs absorbed on major source of HCHs contamination in the study region. SPM from the Jinjiang River was the dominant contribution to the Technical DDT contains higher than 85% of p,p0-DDT and less OCPs pollution in the sediment of Quanzhou Bay. Moreover, this than 15% of o,p0-DDT (Zheng et al., 2009). After technical DDT was might also be attributed to the movement of the seawater to the banned in China from 1983, dicofol (three to seven percent DDTs) Jinjiang River which makes an even mixture of the OCPs in SPM was widely used as another useful acaricide. For p,p0-DDT can and sediment with resuspension. degrade to p,p0-DDE in aerobic environment and to p,p0-DDD in anaerobic environment, the ratios of p,p0-(DDEþDDD)/DDT and p,p0- DDE/DDD are useful to trace the degree of DDT decomposition, as 3.5. Ecological risk assessment well as the environment of decomposition, and to identify the new input of DDT (Lee et al., 2001). The high ratio of p,p0-(DDEþDDD)/ According to the Guidelines of Chinese Environmental Quality DDT (41) suggests aged DDT is the main source, whereas if less Standard for Soils (GB15618-1995), the concentrations of HCHs than 1, the main source is the input of fresh DDTs (Jaga and and DDTs in all samples were both lower than the first grade Dharmani, 2003). The ratio of o,p0-DDT/ p,p0-DDT can show the (50 ng/g for HCHs and 50 ng/g for DDTs). Compared with Dutch contamination from the usage of technical DDT or dicofol (Li et al., target values (NMH 2001), the concentrations of HCHs were all 2008). Generally, the ratio of o,p0-DDT/p,p0-DDT is in the range of lower than the first grade (10 ng/g). But the residues of DDTs 0.2–0.3 in technical DDT and higher than 1.3 in dicofol (Qiu et al., exceeded the first grade (10 ng/g) at four sites in JRW and three 2005). These ratios about this study were shown in Fig.3. sites in QBC. Therefore, the DDT levels might have a potential Here, the ratios of p,p0-(DDEþDDD)/DDT were found less than ecological risk. 1 except in the soil of JRW, suggesting historical application of The concentrations of HCHs and DDTs in water samples technical DDT in the soil of JRW and the fresh input of DDTs in (concentration of DP plus SPM) of the Jinjiang River were other researched environmental media. The ratios of o,p0-DDT/ 12.64–31.53 and 26.28–36.96 ng/L, respectively, which were p,p0-DDT were higher than 1.3 in water and sediment, indicating two orders of magnitude less than the environment quality the dominant dicofol pollution in water of the Jinjiang River and standard for surface water of Chinese guideline (GH ZB1-1999) sediment of Quanzhou Bay. This ratio was less than 1.3 but (o5000 ng/L for HCHs and,o1000 ng/L for DDTs). For European higher than 0.3 in the soil of study areas, which revealed the Union, 20 ng/L of HCHs and 25 ng/L of DDTs were set as environ- possible technical DDT input except the dicofol pollution. The mental quality standard applicable to surface water (2000/60/EC). p,p0-DDE/DDD ratios were more than 1 in the JRW, QBC and SPM, Except J5 (31.53 ng/L), the concentrations of HCHs in water but below 1 in DP, SS and SSS, which reflected relative aerobic samples of the Jinjiang River were slightly lower than the condition in the soil and SPM of water, and anaerobic environ- standard value (20 ng/L). But DDTs in all samples were higher ment in DP of the Jinjiang River and sediment along the than the guideline (25 ng/L), indicated that DDT residues might Quanzhou Bay. have an ecological risk. Table 4 summarized the Pearson’s bivariate correlations of Potential ecotoxicological risk of OCPs residues in sediment of OCPs between different environmental media. The significant Quanzhou Bay was evaluated by comparing with the threshold correlations were shown between the OCPs of SPM and sediment effects level (TEL) and probable effects level (PEL) guidelines (CCME (Canadian Council of Ministers of the Environment), 2002), as well as the effects range-low value (ERL) and effects range-median value (ERM) guidelines (Long et al., 1998; Long and MacDonald, 1995). Table 4 Table 5 shows the concentrations of p,p0-DDE were lower than the Correlations of OCPs between different environmental media. guideline values, while the concentration of g-HCH and p,p0-DDD Media JRW QBC DP SPM SS SSS exceeded the TEL value only at one site. The concentration of DDT (o,p0- and p,p0-DDT) were higher than TEL, PEL and ERL values in JRW 1.000 most of sites, which suggested that the concentration levels of DDT QBC 0.706 1.000 might cause adverse biological risk. For DDTs, although not exceed DP 0.558 0.423 1.000 SPM 0.649 0.510 0.054 1.000 than PEL value, most sample sites were higher than TEL and ERL SS 0.677 0.524 0.095 0.996nn 1.000 values, suggesting that the exposure of DDTs may cause ecological SSS 0.618 0.502 0.036 0.985nn 0.986nn 1.000 risk on the neighboring benthic organisms. Therefore, DDTs could be the specie of OCPs with more ecotoxicological concern in nn Correlation is significant at the 0.01 level (two-tailed). Quanzhou Bay.

Table 5 Comparison between OCP levels in surface sediments of Quanzhou Bay and guideline values (dry weight (ng/g)).

Chemical Range (ng/g) TELa Above TELb PELc Above PELb ERLd Above ERLb ERMe Above ERMb

g-HCH n.d.f–0.43 0.32 1 0.99 0 – – o,p0-and p,p0-DDT 0–6.60 1.19 7 4.77 5 1 7 7 0 p,p0-DDE 0.11–1.30 2.07 0 3.74 0 2.2 0 27 0 p,p0-DDD 0.07–1.51 1.22 1 7.81 0 2 0 20 0 DDTs 0.21–7.83 3.89 6 51.7 0 1.58 7 46.1 0

a Threshold effect level. b Number of samples above the corresponding levels. c Probable effect level. d Effect range-low value. e Effect range-median value. f Not detected. 64 D. Yang et al. / Ecotoxicology and Environmental Safety 89 (2013) 59–65

4. Conclusions Gong, X.Y., Qi, S.H., Wang, Y.X., Julia, E.B., Lv, C.L., 2007. Historical contamination and sources of organochlorine pesticides in sediment cores from Quanzhou Bay, Southeast China. Mar. Pollut. Bull. 54, 1434–1440. In this study the distribution and contamination status of OCPs Hong, S.H., Yim, U.H., Shim, W.J., Oh, J.R., Viet, P.H., Park, P.S., 2008. Persistent in different environmental media have been studied. Among organochlorine residues in estuarine and marine sediments from Halong Bay, DDTs, o,p0-DDT and p,p0-DDE were dominant in surface soil of Hai Phong Bay, and Balat Estuary, Vietnam. Chemosphere 72, 1193–1202. 0 Hu, L.M., Zhang, G., Zheng, B.H., Qin, Y.W., Lin, T., Guo, Z.G., 2009. Occurrence and JRW, while p,p -DDT was dominant in QBC. The concentration of distribution of organochlorine pesticides (OCPs) in surface sediments of the HCHs in the DP accounted for 55–94% of the total HCHs, while the Bohai Sea, China. 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