2015 9, 22(5): 994 1006 Journal of Fishery Sciences of China 研究论文 DOI: 10.3724/SP.J.1118.2015.14545 1, 于紫玲 2, 林钦 1, 谷阳光 1, 杜飞雁 1 1, 柯常亮 1.,,, 510300; 2., 201306 摘要 : 24 (PAHs), PAHs 191~548 ng/g(, ) 348~460 ng/g 337~518 ng/g 380~491 ng/g, 349.2 ng/g 420.9 ng/g 424.3 ng/g 455.9 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 : 1005 8737 (2015)05 0994 13 (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 19.0~933.90 ng/g [2, 8], PAHs, PAHs, PAHs 收稿日期 : 2014-12-22; 修订日期 : 2015-02-11. 基金项目 : (2014A030310220); (nybjg201204); ()(2012TS15). 作者简介 : (1989 ),,. E-mail: zlingyu@yeah.net 通信作者 :,. E-mail: linqinscs@21cn.com
5 : 995 2~10 [9 10], PAHs 1 1.1,,, ( 1), [11],,, 2014 3,,,, [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.. 1 / 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, 150 1.3 [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, 25550 d; CF, 10 6 mg/ng 1.4 IBM SPSS 18.0 Origin 8.5 One-way ANOVA q PAHs, i
996 22
5 : 997 P<0.05 1.5,, 79%~121%, 0.65%~10.4% 2 2.1 PAHs 24 PAHs ( 2, 2), 15 PAHs 191~548 ng/g (, ), 349.2 ng/g; 348~460 ng/g, 420.9 ng/g; 337~518 ng/g, 424.3 ng/g; 380~491 ng/g, 455.9 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.
998 22 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 1.95 3.91 2.62 2.39 6.43 3.86 2.31 5.99 3.53 2.74 3.76 3.11 AC 23.2 207 53.7 44.3 196 99.4 37.8 59.9 50.8 50.1 62.2 53.8 FL 72.8 169 100.3 60.6 145 101.8 118 165 136 131 148 139.4 PHE 52.4 237 116.2 122 146 133.1 97.0 142 116.6 90.7 167 133.6 AN 5.56 23.5 10.9 6.64 14.0 9.91 4.90 13.6 8.70 7.00 19.7 12.7 FA 5.63 13.4 8.28 7.74 10.9 9.33 8.98 12.6 10.6 9.46 12.0 10.7 PY 13.8 99.8 44.9 22.4 64.5 46.1 33.3 117 80.0 47.1 136 81.9 [a] BaA 0.78 1.55 1.12 1.19 2.15 1.68 1.27 2.28 1.64 1.25 1.84 1.53 CHR 1.32 2.18 1.72 1.75 3.57 2.70 2.01 3.30 2.49 2.54 5.33 3.41 [b] BbFA 4.62 8.64 6.30 7.98 9.24 8.59 6.64 12.4 9.26 7.71 17.2 10.1 [k] BkFA 1.41 3.40 2.44 1.93 4.03 3.20 2.78 4.71 3.60 2.97 7.96 4.56 [a] BaP ND 0.53 0.06 ND 0.87 0.29 ND 1.15 0.48 ND 0.73 0.18 [a, h] DBahA ND 1.01 0.37 ND 1.17 0.39 ND 1.13 0.49 0.50 0.74 0.64 [1, 2, 3-cd] IP ND 0.37 0.10 ND ND ND 0.76 0.13 ND 0.15 0.04 [g, h, i] 苝 BghiP ND 0.42 0.15 0.29 0.85 0.57 ND 0.36 0.12 ND 0.50 0.23 15 PAHs 191 548 349.2 348 460 420.9 337 518 424.3 380 491 455.9 3 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.
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 10 15 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,, 2.5 2.5.1 [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)
1000 22 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 25 16 ** GC-MS-MS [12] Adriatic Sea, Italy 13 16.52 63.33 * HPLC [20] Bahia Blanca Estuary, Argentina 17 1095 GC [18] Persian Gulf 9 91.32 1154.45 HPLC [21] Busan market, Korea 16 12.3 243 GC-MS [22] Victoria Harbour, Hong Kong 15 1050 4260 GC [23] Pearl River, South China 16 1.91 224.03 * GC-MS [24] Dapeng Bay, Shenzhen 16 98.21 251.90 * GC-MS [25] Zhanjiang mangrove areas 15 191 548(74.6 155) * GC-MS the study San Francisco estuary 25 184 6899 GC-MS [19] Mississippi Gulf Coast 25 34 ** GC-MS-MS [12] Adriatic Sea, Italy 13 34.73 * HPLC [20] Bahia Blanca Estuary, Argentina 17 348 1597 GC [18] Busan market, Korea 16 25.9 86.1 GC-MS [22] Dapeng Bay, Shenzhen 16 109.94 161.27 * GC-MS [25] Zhanjiang mangrove areas 15 380 491(81.5 121) * GC-MS the study Adriatic Sea, Italy 13 15.80 * HPLC [20] Mississippi Gulf Coast 25 42 ** GC-MS-MS [12] Busan market, Korea 16 19.0 57.4 GC-MS [22] Dapeng Bay, Shenzhen 16 78.87 165.91 * GC-MS [25] Zhanjiang mangrove areas 15 337 518(86.8 94.3) * GC-MS the study Atlantic Ocean 16 26.9 58.6 * LC [26] Adriatic Sea, Italy 13 14.74 * HPLC [20] cephalopoda Busan market, Korea 16 24.2 81.1 GC-MS [22] Zhanjiang mangrove areas 15 348 460(73.7 101) * GC-MS the study : * ; **(). Note: * means wet weight; ** means mean value (wet weight). 2.5.2 [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) 2.5.3 PAHs (2) PAHs, 57.4 g/d 66.6 g/d ( 5) [30], PAHs 3.07 10 6 ~6.15 10 6, 4.57 10 6 ; PAHs 4.54 10 6 ~
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 0.001 CHR* 0.0044 AC 0.001 BbFA* 0.167 FL 0.001 BkFA* 0.02 PHE 0.001 BaP* 1 AN 0.01 IP* 0.055 FA 0.001 DBahA* 1.11 PY 0.001 BghiP 0.01 BaA* 0.145 : * 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 0.44 3.07 10 6 Ilisha melastoma 93.9 0.17 0.84 5.87 10 6 魟 Dasyatis akajei 96.7 ND 0.59 4.12 10 6 鰶 Konosirus punctatus 118 ND 0.68 4.75 10 6 Osteomugil ophuyseni 74.6 ND 0.71 4.96 10 6 fish Megalops cyprinoides 115 ND 0.88 6.15 10 6 cephalopoda crustaceans Cynoglossus puncticeps 90.1 ND 0.61 4.26 10 6 Sardinella jussieu 155 ND 0.51 3.56 10 6 Parupeneus ciliatus 102 ND 0.69 4.82 10 6 Scatophagus argus 81.4 ND 0.64 4.47 10 6 Johnius belangerii 126 ND 0.61 4.26 10 6 Sepia pharaonis 101 ND 0.56 4.54 10 6 Loligo tagoi 73.7 ND 0.59 4.78 10 6 Loligo chinensis 99.8 0.19 0.72 5.83 10 6 Penaeus penicillatus 89.0 ND 0.68 5.51 10 6 Trachypenaeus curvirostris 94.3 0.19 0.83 6.73 10 6 Parapenaeopsis hardwickii 89.4 ND 0.58 4.70 10 6 Oratosquilla oratoria 86.8 ND 0.72 5.83 10 6 蟳 Charybdis feriatus 87.7 0.21 0.71 5.75 10 6 Portunus sanguinolentus 93.0 0.20 0.76 6.16 10 6 Paphia undulata 81.5 ND 0.92 7.45 10 6 shellfish Meretrix lyrata 121 0.18 0.85 6.89 10 6 Mimachlamys nobilis 118 ND 0.74 6.00 10 6 Ostrea rivaris 94.8 ND 0.62 5.02 10 6 : ND. Note: ND means not detected.
1002 22 5.83 10 6, 5.05 10 6 ; 4.70 10 6 ~6.73 10 6, 5.78 10 6 ; 5.02 10 6 ~ 7.45 10 6, 6.34 10 6 4 PAHs (P<0.05)> > 3 3.1 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
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1006 22 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 510300, China; 2. College of Marine Sciences, Shanghai Ocean University, Shanghai 201306, 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 191 548 ng/g (dry weight), 348 460 ng/g, 337 518 ng/g, and 380 491 ng/g, respectively, and their average levels were 349.2 ng/g, 420.9 ng/g, 424.3 ng/g, and 455.9 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. E-mail: linqinscs@21cn.com