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1 2015 9, 22(5): Journal of Fishery Sciences of China 研究论文 DOI: /SP.J , 于紫玲 2, 林钦 1, 谷阳光 1, 杜飞雁 1 1, 柯常亮 1.,,, ; 2., 摘要 : 24 (PAHs), PAHs 191~548 ng/g(, ) 348~460 ng/g 337~518 ng/g 380~491 ng/g, ng/g ng/g ng/g ng/g PAHs, :, PAHs, 3 PAHs, (BaP), PAHs (<10 5 ) : ; ; ; 中图分类号 : X171 文献标志码 : A 文章编号 : (2015) (polycyclic aromatic hydrocarbons, PAHs) 2 2,,,,, [1 2], PAHs,, [3 5] Yang [5] PAHs, 27.4~275.4 ng/g, PAHs,,, PAHs,, ;,, 2014, 157.3, 1.07 t [6], 2013 [7], ;,, PAHs 19.0~ ng/g [2, 8], PAHs, PAHs, PAHs 收稿日期 : ; 修订日期 : 基金项目 : (2014A ); (nybjg201204); ()(2012TS15). 作者简介 : (1989 ),,. [email protected] 通信作者 :,. [email protected]

2 5 : 995 2~10 [9 10], PAHs 1 1.1,,, ( 1), [11],,, ,,,, [12] 20, 4 24 ( 1) 1.2 [13] Fig. 1 1 Sampling areas for marine organisms in mangrove areas of Zhanjiang 5.00 g, / 2 60% ( 3 cm 3 cm 3 cm ), 40 ml 45 ml /(4.. 1), 1 ml, : Agilent 7890A- 5975C - (GC-MS), HP-5MS (30 m 0.32 mm 0.25 μm); 290 ; ( >99.999%),, 1.3 ml/min;, 1 μl; : 50 1 min, 20 /min 100 ; 10 /min 210, 1 min; 5 /min 290, 5 min : (SIM), (EI), 70 ev, 230, 280, [a] ( BEC, ng/g) : BEC n = å C TEF (1) i i i i= 1, C i PAHs i [ng/g ()]; TEF i i PAHs USEPA [14], : BEC IR EF ED SF CF ILCR = (2) BW AT, ILCR ; IR (g/d); EF (365 d/a); ED (a), 70 a; SF [a], 7.3 mg/(kg d) 1 ; BW, 60 kg; AT, d; CF, 10 6 mg/ng 1.4 IBM SPSS 18.0 Origin 8.5 One-way ANOVA q PAHs, i

3 996 22

4 5 : 997 P< ,, 79%~121%, 0.65%~10.4% PAHs 24 PAHs ( 2, 2), 15 PAHs 191~548 ng/g (, ), ng/g; 348~460 ng/g, ng/g; 337~518 ng/g, ng/g; 380~491 ng/g, ng/g 4, PAHs,, ;, PAHs (P<0.05), PAHs, PAHs 鰶 >> > 魟 >; >; 蟳 > > >; >,, PAHs (384.1 ng/g), (363.8 ng/g), (313.1 ng/g) 2.2 PAHs PAHs 3 PAHs, 3 PAHs(ACL AC FL PHE AN) 73.9%~86.7%( 81.1%, ) 79.2%~ 88.7%(82.4%) 69.3%~83.4%(74.5%) 66.6%~80.8% (75.3%), 4 PAHs(PY BaA CHR) 11.2%~23.7%(16.0%) 8.14%~17.8%(14.5%) 13.7%~27.4%(22.0%) 16.1%~30.8%(21.1%), 5~6 2 PAHs () F1: ; F2: ; F3: 魟 ; F4: 鰶 ; F5: ; F6: ; F7: ; F8: ; F9: ; F10: ; F11: ; Ceph1: ; Ceph2: ; Ceph3: ; Crust1: ; Crust2: ; Crust3: ; Crust4: ; Crust5: ; Crust6: ; SF1: ; SF2: ; SF3: ; SF4:. Fig. 2 Concentrations of PAHs in marine organisms from mangrove areas of Zhanjiang (dry weight basis) F1: Muraenesox cinereus; F2: Ilisha melastoma; F3: Dasyatis akajei; F4: Konosirus punctatus; F5: Osteomugil ophuyseni; F6: Megalops cyprinoides, F7: Cynoglossus puncticeps; F8: Sardinella jussieu; F9: Parupeneus ciliatus; F10: Scatophagus argus; F11: Johnius belangerii; Ceph1: Sepia pharaonis; Ceph2: Loligo tagoi; Ceph3: Loligo chinensis; Crust1: Penaeus penicillatus; Crust2: Trachypenaeus curvirostris; Crust3: Parapenaeopsis hardwickii; Crust4: Oratosquilla oratoria; Crust5: Charybdis feriatus; Crust6: Portunus sanguinolentus; SF1: Paphia undulata ; SF2: Meretrix lyrata; SF3: Mimachlamys nobilis; SF4: Ostrea rivaris.

5 ring number 3 3-rings 4 4-rings 5 5-rings 6 6-rings Tab. 2 表 2 湛江红树林海域生物体中 PAHs 含量水平 Concentrations of PAHs in marine organisms from mangrove areas of Zhanjiang ng g 1 dry weight PAHs PAHs compound : ND. Note: ND means not detected. range fish cephalopoda crustaceans shellfish average range average range average range average ACL AC FL PHE AN FA PY [a] BaA CHR [b] BbFA [k] BkFA [a] BaP ND ND ND ND [a, h] DBahA ND ND ND [1, 2, 3-cd] IP ND ND ND ND ND [g, h, i] 苝 BghiP ND ND ND PAHs PAHs F1: ; F2: ; F3: 魟 ; F4: 鰶 ; F5: ; F6: ; F7: ; F8: ; F9: ; F10: ; F11: ; Ceph1: ; Ceph2: ; Ceph3: ; Crust1: ; Crust2: ; Crust3: ; Crust4: ; Crust5: 蟳 ; Crust6: ; SF1: ; SF2: ; SF3: ; SF4:. Fig. 3 Composition patterns of PAHs in marine organisms from mangrove areas of Zhanjiang F1: Muraenesox cinereus; F2: Ilisha melastoma; F3: Dasyatis akajei; F4: Konosirus punctatus; F5: Osteomugil ophuyseni; F6: Megalops cyprinoides, F7: Cynoglossus puncticeps; F8: Sardinella jussieu; F9: Parupeneus ciliatus; F10: Scatophagus argus; F11: Johnius belangerii; Ceph1: Sepia pharaonis; Ceph2: Loligo tagoi; Ceph3: Loligo chinensis; Crust1: Penaeus penicillatus; Crust2: Trachypenaeus curvirostris; Crust3: Parapenaeopsis hardwickii; Crust4: Oratosquilla oratoria; Crust5: Charybdis feriatus; Crust6: Portunus sanguinolentus; SF1: Paphia undulata ; SF2: Meretrix lyrata; SF3: Mimachlamys nobilis; SF4: Ostrea rivaris.

6 5 : 999 PAHs(BbFA BkFA BaP IP DBahA BghiP) 1.40%~5.24%(2.86%) 2.93%~3.18%(3.01%) 2.93%~3.60%(3.27%) 2.54%~ 6.75%(3.63%) q, 3 PAHs (P<0.05);, 4 PAHs (P<0.05); 5~6 PAHs 4 (P>0.05),, 3 PAHs, 66.7%~88.7%; 4 PAHs, 8.14%~30.9%; 5~6 PAHs, 1.40%~6.75% 2.3 PAHs, PHE/AN [1, 16] AN/(AN+ PHE) [17] FA/(FA+PY) [18] BaA/(BaA+CHR) [19], PAHs, PHE/AN BaA/ (BaA+CHR) PAHs, 4 PHE/AN PHE/AN 7.84~19.79, (PHE/AN>15) 33.3%, (PHE/AN<10) 37.5%, (29.2%) BaA/(BaA+CHR) 0.25~0.45, [BaA/(BaA+ 4 PHE/AN BaA/(BaA+CHR) Fig. 4 Isomeric ratios of PHE/AN and BaA/(BaA+CHR) in marine organisms from mangrove areas of Zhanjiang CHR)>0.35] 87.5%, [0.2<BaA/ (BaA+CHR)<0.35], PHE/AN BaA/ (BaA+CHR), PAHs 2.4 PAHs PAHs, PAHs 3 PAHs [12, 18 26],,, PAHs [23] [21] [18], [24] [25], [12] [20] [22] ; PAHs [19] [18],,, PAHs PAHs, ; PAHs [26], PAHs,, [a] [a] (BaP),,, [a], No.208/2005 [27] [a], [a] 2 ng/g(, ) 5 ng/g 10 ng/g, BaP, 0.17 ng/g (, ) ( 5); BaP, 0.19 ng/g; 蟳 BaP, 0.19 ng/g 0.21 ng/g 0.20 ng/g; BaP, 0.18 ng/g BaP (P>0.05)

7 species fish shellfish Tab. 3 crustaceans 表 3 湛江红树林海域生物体中 PAHs 含量与国内外比较 Comparison of PAHs levels in marine organisms from Zhanjiang mangrove areas with other locations research region PAHs number of PAHs compounds tested PAHs /(ng g 1 ) PAHs content analysis method reference Mississippi Gulf Coast ** GC-MS-MS [12] Adriatic Sea, Italy * HPLC [20] Bahia Blanca Estuary, Argentina GC [18] Persian Gulf HPLC [21] Busan market, Korea GC-MS [22] Victoria Harbour, Hong Kong GC [23] Pearl River, South China * GC-MS [24] Dapeng Bay, Shenzhen * GC-MS [25] Zhanjiang mangrove areas ( ) * GC-MS the study San Francisco estuary GC-MS [19] Mississippi Gulf Coast ** GC-MS-MS [12] Adriatic Sea, Italy * HPLC [20] Bahia Blanca Estuary, Argentina GC [18] Busan market, Korea GC-MS [22] Dapeng Bay, Shenzhen * GC-MS [25] Zhanjiang mangrove areas ( ) * GC-MS the study Adriatic Sea, Italy * HPLC [20] Mississippi Gulf Coast ** GC-MS-MS [12] Busan market, Korea GC-MS [22] Dapeng Bay, Shenzhen * GC-MS [25] Zhanjiang mangrove areas ( ) * GC-MS the study Atlantic Ocean * LC [26] Adriatic Sea, Italy * HPLC [20] cephalopoda Busan market, Korea GC-MS [22] Zhanjiang mangrove areas ( ) * GC-MS the study : * ; **(). Note: * means wet weight; ** means mean value (wet weight) [a] [a] (BaP eq ) (1), 7 PAHs EPA [28], 8 Nisbet [29] ( 4) [a] (BaP eq ) PAHs, 5 [a] 0.44~0.88 ng/g(, ), 0.65 ng/g; BaP eq 0.56 ~0.72 ng/g, 0.62 ng/g; BaP eq 0.58~0.83 ng/g, 0.71 ng/g; BaP eq 0.62~ 0.92 ng/g, 0.78 ng/g, BaP :, BaP eq (P<0.05) PAHs (2) PAHs, 57.4 g/d 66.6 g/d ( 5) [30], PAHs ~ , ; PAHs ~

8 5 : 1001 Tab. 4 表 4 PAHs 各组分的 BaP 毒性当量因子 BaP toxicity equivalency factors (TEFs) for PAHs eompounds PAHs PAHs compound TEFs toxicity equivalency factor PAHs PAHs compound TEFs toxicity equivalency factor ACL CHR* AC BbFA* FL BkFA* 0.02 PHE BaP* 1 AN 0.01 IP* FA DBahA* 1.11 PY BghiP 0.01 BaA* : * PAHs. Note: * means carcinogenic PAHs. Tab. 5 表 5 湛江红树林海域生物体中苯并 [a] 芘等效浓度 (BaP eq ) 和 PAHs 致癌风险水平 BaP equivalent concentration and cancer risk levels of PAHs in marine organisms from mangrove areas of Zhanjiang species PAHs /(ng g 1 ) PAHs concentration BaP BaP concentration BaP BaP equivalent concentration cancer risk level Muraenesox cinereus 91.6 ND Ilisha melastoma 魟 Dasyatis akajei 96.7 ND 鰶 Konosirus punctatus 118 ND Osteomugil ophuyseni 74.6 ND fish Megalops cyprinoides 115 ND cephalopoda crustaceans Cynoglossus puncticeps 90.1 ND Sardinella jussieu 155 ND Parupeneus ciliatus 102 ND Scatophagus argus 81.4 ND Johnius belangerii 126 ND Sepia pharaonis 101 ND Loligo tagoi 73.7 ND Loligo chinensis Penaeus penicillatus 89.0 ND Trachypenaeus curvirostris Parapenaeopsis hardwickii 89.4 ND Oratosquilla oratoria 86.8 ND 蟳 Charybdis feriatus Portunus sanguinolentus Paphia undulata 81.5 ND shellfish Meretrix lyrata Mimachlamys nobilis 118 ND Ostrea rivaris 94.8 ND : ND. Note: ND means not detected.

9 , ; ~ , ; ~ , PAHs (P<0.05)> > PAHs [31] PAHs [32],, 4 PAHs > >, PAHs, PAHs, PAHs, PAHs, PAHs > > [12, 21, 33], 4 PAHs,,,,,,, [34],, PAHs [35], PAHs, PAHs PAHs 鰶 PAHs (P<0.05); PAHs, (K ow ), PAHs PAHs [25, 36 37], PAHs,, [38] 11 PAHs (r=0.327, P>0.05),, PAHs [21] PAHs > >,, ;, ( 1) PAHs [12, 21], PAHs, PAHs PAHs [21],, PAHs, PAHs PAHs 3.2 PAHs, (2~3 )PAHs (K ow ), ; PAHs K ow,, Bruner [39],, ( 61.5%) ; 10, ( 89.5%) PAHs,, 3 PAHs, PAHs [1], 3 PAHs (P<0.05);, 4 PAHs

10 5 : 1003 (P<0.05), PAHs, PAHs lgk ow <5 (2~4 ), lgk ow >5(5~6 ) [10, 40],,,,,,, 3 PAHs, PAHs, PAHs, PAHs ; PAHs, K ow,, [10] 3.3 PAHs, [a] 蟳 6, 1 ng/g, No. 208/2005 [27], BaP 4 BaP > >, PAHs, PAHs BaP (r=0.087, P>0.05), PAHs USEPA ILCR 10 5, ILCR>10 4 [15, 28] 4 PAHs 10 5,, 致谢 : 本研究生物样品的采集和鉴定得到南海水产研究所王雪辉副研究员 宁加佳老师 李亚芳 老师 王亮根老师等的帮助, 特致谢忱! 参考文献 : [1] Shahbazi A, Zakaria M P, Yap C K, et al. Spatial distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in green mussels (Perna viridis) from coastal areas of Peninsular Malaysia: implications for source identification of perylene[j]. Int J EnvironAnal Chem, 2010, 90(1): [2] Huang W, Wang Z, Yan W. Distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in sediments from Zhanjiang Bay and Leizhou Bay, South China[J]. Mar Poll Bull, 2012, 64(9): [3] Ding X, Xie Z Q, Xiang C H, et al. Observed latitudal distribution of gaseous polycyclic aromatic hydrocarbons aboard Xuelong during chinare 2003[J]. Chinese Journal of Polar Research, 2005, 17(4): [,,, [J]., 2005, 17(4): ] [4] Farrington J W, Takada H. Persistent organic pollutants (POPs), polycyclic aromatic hydrocarbons(pahs), and plastics examples of the status, trend, and cycling of organic chemicals of environmental concern in the ocean[j]. Oceanography, 2014, 27(1): [5] Yang G P. Polycyclic aromatic hydrocarbons in the sediments of the South China Sea[J]. Environ Poll, 2000, 108(2): [6]. [N]., [7] South China Sea Branch, State Oceanic Administration. The marine environmental quality status report 2013[EB/OL] [EB/OL]. http: // ] [8] Zhao L R, Sun S L, Ke S. Characteristics of PAHs pollution in sediments from Leizhou coastal marine area, Liusha Bay and Shenzhen Bay[J]. Environmental Science, 2012, 33(4): [,,. PAHs [J]., 2012, 33(4): ] [9] Tam N F Y, Ke L, Wang X H, et al. Contamination of polycyclic aromatic hydrocarbons in surface sediments of mangrove swamps[j]. Environ Poll, 2001, 114(2): [10] Liang Y, Tse M F, Young L, et al. Distribution patterns of polycyclic aromatic hydrocarbons (PAHs) in the sediments and fish at Mai Po Marshes Nature Reserve, Hong Kong[J]. Water Res, 2007, 41(6): [11] Yang S Y, Bao X W, Chen C S, et al. Analysis on character-

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13 Levels and health risk assessment of polycyclic aromatic hydrocarbons in marine organisms from Zhanjiang mangrove waters YU Ziling 1, 2, LIN Qin 1, GU Yangguang 1, DU Feiyan 1, KE Changliang 1 1. Key Laboratory of Fishery Ecology and Environment, Guangdong Province of China; Key Laboratory of South China Sea Fishery Resources Exploitation & Utilization, Ministry of Agriculture; South China Sea Fisheries Research Institute, Chinese Academy of Fishery Sciences, Guangzhou , China; 2. College of Marine Sciences, Shanghai Ocean University, Shanghai , China Abstract: Polycyclic aromatic hydrocarbons (PAHs) are a large group of anthropogenic pollutants that contain two or more fused aromatic rings in linear, angular, or clustered arrangements. PAHs are introduced into marine environments through events such as atmospheric deposition, accidental oil spills, transport accidents, combustion of fuels, municipal, and urban runoff. PAHs elicit particular concern, and 16 PAHs were listed as priority pollutants by the US EPA because of their health risk as potential carcinogens and mutagens. Because of their lipophilic properties and resistance to degradation, PAHs can accumulate in organic tissue. Consequently, alarming concentrations of these compounds have been found in many marine species. Levels, composition profiles, and health risk assessment of PAHs were studied in 24 species of marine organisms collected from Zhanjiang mangroves. PAH concentrations were determined using gas chromatography coupled with mass spectroscopy. The results demonstrated that the total concentration of PAHs in 11 species of marine fishes, 3 species cephalopods, 6 species crustaceans, and 4 species shellfish ranged from ng/g (dry weight), ng/g, ng/g, and ng/g, respectively, and their average levels were ng/g, ng/g, ng/g, and ng/g, respectively. The average PAH concentrations differed among species and in the following decreasing order: shellfish>crustaceans>cephalopods>marine fishes. Compared with PAH levels of other coastal areas of the world, the PAH levels from Zhanjiang mangroves were low to moderate. The composition of PAHs was characterized by three rings of PAHs. Potential risk assessments demonstrated that the levels of benzo[a]pyrene in fishes, cephalopods, crustaceans, and shellfish from Zhanjiang mangroves were within the EU limits and were considered acceptable (<10 5 ). Key words: mangrove areas; marine organism; PAHs; risk assessment Corresponding author: LIN Qin. [email protected]