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2 Marine Pollution Bulletin 76 (2013) Contents lists available at ScienceDirect Marine Pollution Bulletin journal homepage: Baseline Heavy metals distribution and contamination in surface sediments of the coastal Shandong Peninsula (Yellow Sea) Guogang Li a, Bangqi Hu b,, Jianqiang Bi a, Qinuan Leng a, Chunqiao Xiao a, Zhongcheng Yang c a Beihai Offshore Engineering Survey Institute of the State Oceanic Administration, Qingdao , China b Key Laboratory of Marine Hydrocarbon Resources and Environmental Geology, Qingdao Institute of Marine Geology, Ministry of Land and Resources, Qingdao , China c Qingdao Bohai Construction Group Corporation, Qingdao , China article info abstract Keywords: Heavy metals contamination Sediment quality guidelines Environmental assessment Shandong Peninsula Selected heavy metals (Cr, Cu, Ni, Pb and Zn) in surface sediments from the coastal Shandong Peninsula (Yellow Sea) have been determined to evaluate the spatial distribution and potential ecological risk. Results showed that heavy metal concentrations in the sediments generally met the criteria of China Marine Sediment Quality. However, both the enrichment factor (EF) and geoaccumulation index (I geo ) values suggested the elevation of Pb concentration in the region. Based on the effect-range classification (TEL-PEL SQGs), Cr, Cu and Ni were likely to pose environment risks. Spatial distribution of ecotoxicological index (mean-pel-quotient) suggested that most of the surface sediments have a 21% probability of being toxic. Similar results were also obtained by pollution load index (PLI). The spatial distribution pattern of heavy metal in surface sediments is a basis for undertaking appropriate action to protect marine sediment quality. Ó 2013 Elsevier Ltd. All rights reserved. Since 1980s, a rapid industrialization and economic development in China has brought a thriving economic success, accompanied with a series of severe environmental problems (Gao and Chen, 2012; Gu et al., 2012; Pan and Wang, 2012; Zhang et al., 2012b; Gan et al., 2013; Zhao et al., 2013). Toxic pollutants, such as heavy metals originating from human activities, are continuing to be introduced to aquatic environment through rivers, waste dumping and aeolian processes, then deposited in marine sediments as a sink. One of the largest problems associated with the persistence of heavy metals is the potential for bioaccumulation and biomagnification, resulting in potential long-term implications on human health and ecosystem (Rainbow, 2007; Wang and Rainbow, 2008). Due to the toxicity and persistence of heavy metal pollution, heavy metal research of estuarine and coastal area has attracted more public concerns recently (Christophoridis et al., 2009; Larrose et al., 2010; Feng et al., 2011; Liu et al., 2011; Sundaray et al., 2011; Varol, 2011; Gao and Li, 2012; Yang et al., 2012; Hu et al., 2013a; Hu et al., 2013b). It is necessary to investigate the distribution and pollution degree of heavy metal, in order to interpret the mechanism of transportation and accumulation of pollutants and to provide basic information for coast utilization and supervision (Long et al., 1998; Long et al., 2006). Corresponding author. Address: Qingdao Institute of Marine Geology, Fuzhou South Road 62#, Qingdao, Shandong , China. Tel.: ; fax: address: bangqihu@gmail.com (B. Hu). The Shandong Peninsula locates in the eastern China, west coast of the Yellow Sea, separates the South Yellow Sea (SYS) from the North Yellow Sea (NYS). Bedrocks of Shandong Peninsula are mainly igneous and metamorphic rocks. Small rivers (e.g. Dagu, Wulong, Rushan and Muzhu Rivers) originate from peninsula hills and flow into sea from both south and north banks of Shandong Peninsula (Xu et al., 2013a). As a spawning, feeding ground for a variety of marine life and traditional fishing ground, the coastal area around Shandong Peninsula is an important fishery and breeding area in eastern China (Jin and Tang, 1996; Gao et al., 2003). Several big cities (Qingdao, Yantai and Weihai Cities), with millions of population and prosperous economy, are located in the coastal area of Shandong Peninsula. It is part of Bohai economic rim and Yellow River economic belt, one of indispensable part of China s coastal economic belt. Due to the rapidly expanding economic and industrial developments in these cities, anthropogenic pollutants increased obviously, resulting in heavy metal contamination occurring in Shandong Peninsula coastal area in recent decades. For example, Jiaozhou Bay, located in south of Shandong Peninsula and surrounded by Qingdao city, was found heavily polluted for the Cu, Pb, Cd and Zn near estuaries of the east coast (Deng et al., 2010). Heavy metal pollution status of Shandong Peninsula coastal area has attracted considerable attention of both scientific and regulatory communities. Recent studies mainly focused on assessment of heavy metal pollution of some estuaries and bays around Shandong Peninsula (Wang et al., 2007; Gao et al., 2008; Deng et al., 2010; Sun et al., 2012; Zhang et al., 2012a; Sheng X/$ - see front matter Ó 2013 Elsevier Ltd. All rights reserved.

3 G. Li et al. / Marine Pollution Bulletin 76 (2013) et al., 2013; Xu et al., 2013a, 2013b) or the offshore area of South Yellow Sea (He et al., 2008; Yuan et al., 2012). So far, there are limited works focused on large-scale and thoroughly sampled investigation for the coastal area of Shandong Peninsula. In this study, a total of 208 surface sediment samples, collected around the coastal area of Shandong Peninsula, were analyzed for sediment types and chemical composition. Our main objectives are: (1) to reveal the spatial distribution of heavy metals (Cr, Cu, Ni, Pb and Zn) in the study area, (2) to assess potential ecological risk using mean-pel-quotients (M-PEL-Q), (3) to evaluate the metal contamination using the enrichment factor (EF), geoaccumulation index (I geo ) and pollution load index (PLI). Based on Chinese Offshore Investigation and Assessment Project, a total of 208 surface sediment samples (0 2 cm depth) were collected from the coastal Shandong Peninsula (Fig. 1) in All samples were obtained by a stainless steel grab sampler. After determining general sediments characteristics onboard, sediment samples were then frozen in cold store until further laboratory analysis. Bulk sediment sample was divided into three subsamples for the determinations of heavy metals, total organic carbon (TOC) and grain size. Grain size analysis was performed using Malvern Mastersizer 2000 laser particle size analyzer. Before analysis, about 1 g samples were pre-treated with 30% H 2 O 2 and 0.5 N HCl for 24 h to remove organic matter and biogenic carbonate. Prior to elements analyses, about 20 g of the sub-samples were oven-dried at 45 C for 24 h, then ground to pass a mm sieve and stored in clean plastic bags at room temperature. An X-ray fluorescence spectrometer (XRF, Axios PW4400) was used for determining Al and Fe and inductively coupled plasma mass spectrometry (ICP-MS, Thermo X series) for Cr, Cu, Ni, Pb and Zn. Blanks and China Stream Sediment Reference Materials (GSD9, GSD4 and GBW07345) were included in the analyses as part of the quality assurance and quality control (QA/QC) (see Dou et al., 2013 for detail). The differences of the concentrations between the determined and certified values were less than 5%, and the analytical precision for replicate samples was within ±10%. Prior to total organic carbon (TOC) analysis, sub-samples were freeze-dried and pulverized. After that, about 1 g sediments were treated with 10% HCl for 3 h to remove inorganic carbon, then dried and determined with a Carlo-Erba element analyzer. The measurement error was within 5% based on replicate sediment analysis. The statistical summary and other comparisons of the heavy metal contents are summarized in Table 1. The ranges of heavy metal contents and TOC were: mg/kg for Cr, mg/kg for Cu, mg/kg for Ni, mg/kg for Pb, mg/kg for Zn and % for TOC. Based on the mean content, the components in surface sediments were arranged in the following decreasing order: Zn > Cr > Ni > Pb > Cu. Fig. 1. Map showing the Yellow Sea in North China (a) and the surface sampling sites in the coastal Shandong Peninsula (b).

4 422 G. Li et al. / Marine Pollution Bulletin 76 (2013) Table 1 Summary of heavy metal concentrations in surface sediments of the coastal Shandong Peninsula (unit: mg kg 1 ). Regions Cr Cu Ni Pb Zn Reference Coastal Shandong Peninsula This study (57.8 ± 10.7) (20.0 ± 7.2) (31.2 ± 6.5) (28.4 ± 3.7) (74.7 ± 22.4) Bohai Bay, Bohai Sea Hu et al. (2013a) (33.5) (22.7) (30.5) (21.7) (71.7) Liaodong Bay, Bohai Sea Hu et al. (2013b) (46.4) (19.4) (22.5) (31.8) (71.7) Changjiang Estuary Zhang et al. (2009) (78.9) 30.7 (31.8) (27.3) (94.3) Pearl River Estuary Zhou et al. (2004) (89.0) (46.2) (41.7) (59.3) (150) South Yellow Sea n.d n.d Yuan et al. (2012) (16.9) (17.8) (93.7) East China Sea Inner Shelf n.d Liu et al. (2011) (93.5) (37.4) (34.1) (116) Izmit Bay, Turkey n.d Pekey, 2006 Hamer and Karius, 2002 Bremen Bay, Germany Masan Bay, Korea Hyun et al. (2007) (67.1) (43.4) (28.8) (44.0) (206.3) Average upper crust of East China Gao et al. (1998) MSQ-1 a n.d CSBTS (2002) MSQ-2 a n.d CSBTS (2002) a MSQ-1 and MSQ-2 are the Marine Sediment Quality standard criteria (GB ) issued by the China State Bureau of Quality and Technical Supervision (CSBTS). For the comparison purpose, the average upper continental crust (UCC) values of East China (Gao et al., 1998) and other regions throughout the world are listed in Table 1. In surface sediments from the coastal Shandong Peninsula, the mean contents of Cu, Ni and Cr (Pb and Zn) were lower (higher) with respect to their corresponding average values in the UCC of East China (Table 1). Among all the coastal areas chosen for comparison, the average content of Cr for coastal Shandong Peninsula was higher than that of Bohai and Liaodong Bay (Hu et al., 2013a; Hu et al., 2013b) in the Bohai Sea, but much lower than other regions. For the other four selected metals (Cu, Ni, Pb and Zn), the mean contents of coastal Shandong Peninsula were comparable with those of Bohai and Liaodong Bay, but lower than those found in the Changjiang Estuary (Zhang et al., 2009) and Pearl River Estuary (Zhou et al., 2004), where their surrounding areas are the other two most heavily urbanized zones in China. In addition, the average concentrations of Cr, Cu, Ni, Pb and Zn in the study area were significantly lower than those found in sediments of the Izmit Bay in Turkey (Pekey, 2006), Bremen Bay in Germany (Hamer and Karius, 2002) and the Masan Bay in Korea (Hyun et al., 2007). In general, the spatial distribution of heavy metals and TOC show similar patterns (Fig. 2). In the southern Shandong Peninsula, high content zones of heavy metals and TOC are located in the offshore area extending towards northwest, while relative higher content zone are distributed along the nearshore area of the north Shandong Peninsula. Low values of heavy metals and TOC are found nearby the east end of Shandong Peninsula (Chengshan Cape). It is well known that organic matter has a high affinity through adsorption or complexion for heavy metals in the aquatic environment (Dou et al., 2013; Hu et al., 2013a; Hu et al., 2013b). Significant positive correlations between TOC and heavy metals are established (Table 2), suggesting that TOC is an important factor controlling the abundance of heavy metals. Sediment grain size is another controlling factor affecting the abundance of heavy metals in sediments. Due to surface adsorption and ionic attraction, fine-grained sediments tend to have relatively high metal contents. In this study, mean grain size (Mz) was found to be positive correlated with most metals (Table 2), with Pearson s correlation coefficients (r) as 0.51 for Cr, 0.56 for Cu, 0.49 for Pb, 0.38 for Zn, 0.51 for Ni (p < 0.01, n = 208). This suggests that heavy metals contents were influenced by grain size to a certain extent. It is important to determine whether the concentrations of heavy metals in sediments pose a threat to aquatic life. The extent of metal pollution was assessed by comparing metal concentrations in surface sediments to the China Marine Sediment Quality (GB ) (CSBTS, 2002) and the TEL/PEL SQGs (Macdonald et al., 1996; Long et al., 1998; MacDonald et al., 2000). Marine Sediment Quality (GB ), established by China State Bureau of Quality and Technical Supervision (CSBTS, 2002), contains three standard criteria for marine sediments. The primary sediment standard criteria is applied to protecting the habitats for marine life including natural, rare and endangered species as well as the areas for human recreation and sports, while the second sediment standard criteria is applied to regulating general industrial use and coastal tourism. Referring to Marine Sediment Quality (GB ), the overall average concentrations of all selected heavy metals in the coastal Shandong Peninsula surface sediments are below or close to the primary standard criteria (Table 1). However, the metal concentrations at several sampling sites exceeded the primary criteria (MSQ-1). Among the 208 sampling sites, there were eight sites exceeding the primary criteria for Cr, six sites for Cu, and four sites for Zn, but below the secondary criteria (MSQ-2). Because there are no Ni standards available in GB , we cannot evaluate the sediment quality with respect to Ni. In general, the studied five heavy metal concentration suggested that the overall sediment quality in the coastal Shandong Peninsula has not been significantly impacted by heavy metal pollution. The TEL/PEL SQGs are also applied to assess the degree to which the sediment-associated chemical status might adversely affect aquatic organisms and are designed to assist in the interpretation of sediment quality (Macdonald et al., 1996; Long et al., 1998; Mac- Donald et al., 2000). The threshold effects level (TEL) were interpreted to present chemical concentrations below which adverse biological effects rarely occur, and the probable effects level (PEL) were intended to present chemical concentrations above which adverse biological effects frequently occur (Macdonald et al., 2000). When compared to the TEL-PEL SQGs, the concentrations of Cr, Cu, Ni, Pb and Zn are below TEL with 36%, 45%, 0%, 96% and 73% of sample sites, respectively, and 64% for Cr, 55% for Cu, 95% for Ni, 4% for Pb and 27% for Zn fall in the range between TEL and PEL. There are also 5% of sample sites for Ni slightly exceeds PEL, which indicated a potential harm for aquatic organisms (Table 3).

5 G. Li et al. / Marine Pollution Bulletin 76 (2013) Fig. 2. Spatial distribution of total organic carbon (%TOC) and heavy metal concentrations (Cr, Cu, Ni, Pb and Zn, mg kg 1 ) of surface sediments in the coastal Shandong Peninsula. Table 2 Pearson s correlation matrix for the heavy metals and major elements, TOC and mean grain-size (Mz). TOC Mz Cr Cu Pb Zn Ni Al Mz Cr Cu Pb Zn Ni Al Fe Correlation is significant at the 0.01 level (two-tailed). Table 3 Comparison between heavy metals concentration (mg/kg) in the study area and the TEL and PEL-SQGs (MacDonald et al., 2000). Sediment quality guidelines Metal concentration (mg/kg) Cr Cu Ni Zn Pb TEL PEL Compared with TEL and PEL (% of sample in each guideline) <TEL (%) PTEL and < PEL (%) PPEL (%) In order to combine metal-specific SQG values and then to determine the possible biological effect of combined metals, the mean PEL quotients (m-pel-q) for the five measured heavy metals (Cr, Cu, Ni, Pb and Zn) were calculated as following (Long et al., 1998): m PEL Q ¼ X n i¼1 ðc i =PEL i Þ n where C i is the concentration of measured metal (i), PEL i is the PEL values of metal (i) and n is the number of metal. Several classes of toxicity probability for biota were defined as: m-pel-q < 0.1: 8% probability of toxicity; : 21% probability of toxicity; : 49% probability of toxicity; and >2.3: 73% probability of toxicity (Long et al., 1998). The m-pel-q in surface sediments of the coastal Shandong Peninsula varied from 0.22 to 0.62 (mean value of 0.36), indicating that the combination of the five studied metals may have a 21% probability of being toxic. Based on the m- PEL-Q data, a contour map of multi-metals ecological risk potential of east Shandong Peninsula was presented (Fig. 3a). The highest potential ecological risk zone was found in southeast area and relatively high potential was found in the nearshore area of north Shandong Peninsula. The enrichment factor (EF) is widely used to estimates the metal source (anthropogenic or natural) and the degree of anthropogenic influence based on the use of a normalization element in order to alleviate the variations produced by heterogeneous sediments (Adamo et al., 2005). In this study, the crustal average metal concentrations in eastern China (Gao et al., 1998) were used as the background metal values shown in (Table 1). We defined the EF as the sample metal (Me) to aluminum (Al) ratio divided by the baseline metal/al ratio, and expressed as: ð1þ

6 424 G. Li et al. / Marine Pollution Bulletin 76 (2013) (a) 2 EF Cr Cu Ni Pb Zn (b) 0 Igeo Cr Cu Ni Pb Zn (c) 2 CF 1 Fig. 3. Spatial distribution of m-pel-q (a) and PLI (b) in the coastal Shandong Peninsula. 0 Cr Cu Ni Pb Zn EF ¼ ðme=alþ sample ð2þ ðme=alþ baseline where (Me/Al) sample and (Me/Al) baseline represent the ratio of heavy metal to Al concentrations in this study and in background sample, respectively. Generally, an EF value of suggests the given metal may be entirely provided from crustal contribution or natural weathering processes, while the EF value greater than 1.5 indicates a significant proportion of non-crustal metal composition coming from either natural processes or anthropogenic influence (Zhang and Liu, 2002). The EF values of heavy metals in the study area varied as follow: (mean of 0.57) for Cr, (mean of 0.72) for Cu, (mean of 0.84) for Ni, (mean of 1.9) for Pb and (mean of 1.12) for Zn (Fig. 4a). As shown in box and whisker plot (Fig. 4a), the EF values of Cr, Cu, Ni and Zn were less than 1.5, suggesting a primary natural source in the study area, whereas the EF values of Pb were all greater than 1.5, indicating a notably non-crustal origin. This suggests that Pb was the most contaminated element among the five studied heavy metals, and the major source of Pb was anthropogenic input such as gasoline and industrial activities (Cheng and Hu, 2010). The geoaccumulation index (I geo ) is another parameter to assess the heavy metal contamination (Müller, 1979), is defined as the following equation: C n I geo ¼ log 2 ð3þ 1:5B n Fig. 4. Box-and-whisker plots for (a) EF, (b) I geo and (c) CF of heavy metals in the surface sediments of coastal Shandong Peninsula. of the background values due to lithogenic effects (Müller, 1979). A seven-level classification of I geo is defined as: unpolluted (I geo 6 0), unpolluted to moderately polluted (0 < I geo 6 1), moderately polluted (1 < I geo 6 2), moderately to strongly polluted (2 < I geo 6 3), strongly polluted (3 < I geo 6 4), strongly to extremely polluted (4 < I geo 6 5), and extremely polluted (I geo >5) (Müller, 1981). The I geo values of surface sediments from the coastal Shandong Peninsula are 2.08 to 0.58 (average 1.39) for Cr, 2.29 to 0.19 (average 1.12) for Cu, 1.55 to 0.03 (average 0.86) for Ni, 0.24 to 0.91 (average 0.32) for Pb and 1.42 to 0.87 (average 0.46) for Zn, respectively (Fig. 4b). The averaged pollution degree of these metals decreased in the following order: Pb > Zn > Ni > Cu > Cr, which is similar with that observed from EF values. According to the Müller scale (Müller 1981), the I geo values indicates no pollution of the investigated metals in the study area as a whole, although some deviation is observed depending on each metal and sampling location. The I geo values for Pb were between 0 and 1 generally, indicating that slight to moderate Pb pollution occurred around Shandong Peninsula. The contamination factor (CF) and pollution load index (PLI) are also introduced to assess the degree of anthropogenic metal contamination. The CF for each metal is the ratio of measured concentration in the sediment to the background value, which is defined as follows: where C n is the concentration of metal (n) and B n is the geochemical background concentration of metal (n). The factor of 1.5 is a background matrix correction factor that includes possible variations CF ¼ Me sample Me baseline ð4þ

7 G. Li et al. / Marine Pollution Bulletin 76 (2013) If CF < 1, it means no or low contamination exists; 1 < CF < 3 is moderate contamination; 3 < CF < 6 is considerable contamination; and CF > 6 is very high contamination (Hakanson, 1980). The PLI is determined as the nth root of the n contamination factors (CF n ) multiplied together and calculated using the following equation: PLI ¼ðCF 1 CF 2 CF 3... CF n Þ 1=n This empirical index provides a simple, comparative means for assessing the level of heavy metal pollution. The PLI value >1 indicates a polluted condition, while PLI <1 means no metal pollution existing (Tomlinson et al., 1980). The results of CFs are 0.35 to 1.01 (average 0.58) for Cr, 0.25 to 1.71 (average 0.74) for Cu, 1.27 to 2.81 (average 1.89) for Pb, 0.56 to 2.74 (average 1.13) for Zn, 0.51 to 1.53 (average 0.84) for Ni, respectively (Fig. 4c), with the same decreasing order as EF and I geo : Pb > Zn > Ni > Cu > Cr. The PLI values are between 0.56 and 1.62, with mean of Among all sampling sites, 69 of 208 values are greater than 1, which means 33% of sites are metal contaminated to some extent. As shown in the contour map of PLI values (Fig. 3b), the distribution of pollution are the same as that observed from m-pel-q index (Fig. 3a). This field study demonstrated that the sediment quality in the coastal Shandong Peninsula (Yellow Sea) generally met the primary sediment criteria of Chinese Marine Sediment Quality (GB ). Both the EF and I geo values showed a moderate to significant Pb contamination in the study area. In compared with consensus-based SQGs, Cr, Cu and Ni were likely to result in occasionally adverse biological effects on the aquatic ecosystems. Spatial distribution of the ecotoxicological index (mean-pel-quotients) suggests that the combination of the five studied metals may have a 21% probability of being toxic. 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