| 472 | 0 | 246 |
| 下载次数 | 被引频次 | 阅读次数 |
多环芳烃(Polycyclic aromatic hydrocarbons, PAHs)是一类具有强致癌、致畸和致突变效应的持久性有机污染物。在高强度人类活动背景下，近海环境中PAHs的分布、来源和风险评估备受关注。本文通过2022年8月(丰水期)和2023年4月(枯水期)在胶州湾海域开展的2次调查，分析了胶州湾表层海水中PAHs(DPAHs)、悬浮颗粒物中PAHs(PPAHs)和表层沉积物中PAHs(SPAHs)污染状况、来源及介质分配行为，并评估了其生态风险。胶州湾丰水期16种DPAHs、PPAHs和SPAHs的平均浓度分别为(124.7±19.7)、(345.8±141.7)和(634.4±121.9) ng·g-1;枯水期DPAHs和PPAHs的平均浓度分别为(622.5±215.8)和(239.6±313.9) ng·L-1。丰水期DPAHs以3环为主，平均占比为28.1%±4.5%,枯水期以4环为主，平均占比为42.9%±5.3%;丰水期与枯水期PPAHs均以3环为主，平均占比分别为40.5%±6.6%和42.2%±10.4%;SPAHs以2—4环为主，平均占比为84.4%±3.1%。DPAHs和PPAHs与盐度呈显著负相关，表明陆源输入是胶州湾水体中PAHs的重要来源；丰水期PPAHs浓度与颗粒有机碳呈显著正相关，而2环SPAHs与沉积有机碳呈显著正相关，表明有机碳含量是影响PPAHs和SPAHs分布的重要因素。丰水期和枯水期16种PAHs的颗粒物-水有机碳归一化系数的对数(lgK_(OC(SPM-W)))大部分低于经典平衡分配模型的预测值下限且与辛醇-水分配系数的对数(lgKOW)之间的斜率小于1,表明胶州湾颗粒物对PAHs的亲和力较差。特征比值解析结果表明，胶州湾PAHs主要来源于石油、煤炭、生物质燃烧。胶州湾DPAHs丰水期为低风险，枯水期为中高风险；PPAHs在丰水期和枯水期均为中低风险；SPAHs则为中高风险。
Abstract：Polycyclic Aromatic Hydrocarbons(PAHs) are a class of persistent organic pollutants(POPs) with carcinogenic, teratogenic and mutagenic. Under the background of high-intensity human activities, the distribution, sources and risk assessment of PAHs in the offshore are of great concern. Based on two surveys conducted in August 2022(wet season) and April 2023(dry season) in Jiaozhou Bay, this paper analyzes the pollution status, sources and distribution behaviors amongdifferent media in surface seawater(DPAHs), PAHs in suspended particulate matter(PPAHs) and PAHs in surface sediment(SPAHs), and assesses the ecological risk of PAHs. During the wet season, the average concentrations of DPAHs, PPAHs and SPAHs are(124.7±19.7),(345.8±141.7) and(634.4±121.9) ng·g-1 dw, respectively. The mean concentrations of DPAHs and PPAHs are(622.52±215.8) and(239.6±313.9) ng·L-1 in the dry season, respectively. DPAHs are dominated by 3 rings in the wet season, with an average proportion of 28.1%±4.5% and are dominated by 4 rings in the dry season, with an average proportion of 42.9%±5.3%. In both the wet and dry seasons, PPAHs are dominated by 3 rings, with an average proportion of 40.49%±6.63% and 42.23%±10.42%, respectively. SPAHs are dominated by 2—3 rings, with an average percentage of 67.5%±7.0%. DPAHs and PPAHs show a significant negative correlation with salinity, indicating that land-based input is an important source of PAHs in waterof Jiaozhou Bay. The significant positive correlation between PPAHs and POC, 2 rings SPAHs and TOC in the wet season, indicating that the content of organic matter is the important factors influencing the distribution of PPAHs and SPAHs. The logarithm of the normalized particulate-water organic carbon coefficients(lgK_(OC(SPM-W))) for the 16 PAHs inthewetanddryseasonsare mostly lower than the lower limit of the predictions of the classical equilibrium partitioning model and the slopes with respect to the logarithm of the partition coefficients of the octanol-water(lgKOW) are less than 1, suggesting that the particulate matter of the Jiaozhou Bay has a poor affinity for PAHs. The results of PAHs characterization ratio analysis indicatethat oil, coal, and biomass combustion are the main sources of PAHsin Jiaozhou Bay. DPAHs are low risk in the wet season and medium-high risk in the dry season. PPAHs are medium-low risk during both the wet and dry seasons, and SPAHs are medium-high risk.
[1] Wang Y,Wang J Y,Mu J L,et al.Aquatic predicted no-effect concentration for three polycyclic aromatic hydrocarbons and probabilistic ecological risk assessment in Liaodong Bay of the Bohai Sea,China[J].Environmental Science and Pollution Research,2014,21(1):148-158.
[2] Yu Z,Lin Q,Gu Y,et al.Spatial-temporal trend and health implications of polycyclic aromatic hydrocarbons (PAHs) in resident oysters,South China Sea:A case study of Eastern Guangdong coast[J].Marine Pollution Bulletin,2016,110(1):203-211.
[3] Yim U,Hong S,Ha S,et al.Source and region specific distribution of polycyclic aromatic hydrocarbons in sediments from Jinhae Bay,Korea[J].Science of the Total Environment,2014,470:1485-1493.
[4] Shi W T,Xu M,Liu Q,et al.Polycyclic aromatic hydrocarbons in seawater,surface sediment,and marine organisms of Haizhou Bay in Yellow Sea,China:Distribution,source apportionment,and health risk assessment[J].Marine Pollution Bulletin,2022,174:113280.
[5] Qian X,Liang B C,Fu W J,et al.Polycyclic aromatic hydrocarbons (PAHs) in surface sediments from the intertidal zone of Bohai Bay,Northeast China:Spatial distribution,composition,sources and ecological risk assessment[J].Marine Pollution Bulletin,2016,112(1-2):349-358.
[6] Qian Y,Wade T L,Sericano J L.Sources and bioavailability of polynuclear aromatic hydrocarbons in Galveston Bay,Texas[J].Estuaries,2001,24(6):817-827.
[7] Gonul L T,Kucuksezgin F.Aliphatic and polycyclic aromatic hydrocarbons in the surface sediments from the Eastern Aegean:Assessment and source recognition of petroleum hydrocarbons[J].Environmental Science and Pollution Research,2012,19(1):31-41.
[8] Jia X M,Li J Y,Tian S Y.Assessment of polycyclic aromatic hydrocarbons (PAHs) ecological risk in surface seawater from the west Bohai Bay,China[J].IOP Science,2017,82(1):012040.
[9] Oyo-Ita I,Nkom P Y,Ugim S U,et al.Seasonal changes of PAHs in water and suspended particulate matter from Cross River Estuary,SE Nigeria in response to human-induced activity and hydrological cycle[J].Polycyclic Aromatic Compounds,2022,42(8):5456-5473.
[10] Yin Z Y,Li J S,Huang J,et al.Steady increase in water clarity in Jiaozhou Bay in the Yellow Sea from 2000 to 2018:Observations from MODIS[J].Journal of Oceanology and Limnology,2021,39(3):800-813.
[11] 韩彬，辛明，陈发荣，等.胶州湾东北部海域生态环境污染状况研究[J].岩矿测试，2009,28(6):524-528.Han B,Xin M,Chen F R,et al.Studyon ecological environment pollution status in the sea areas of northeastern Jiaozhou Bay[J].Rock and Mineral Analysis,2009,28(6):524-528.
[12] 王江涛，谭丽菊，张文浩，等.青岛近海沉积物中多环芳烃、多氯联苯和有机氯农药的含量和分布特征[J].环境科学，2010,31(11):2713-2722.Wang J T,Tan L J,Zhang W H,et al.Concentrations and distribution characteristic of PAHs,PCBs and OCPs in the surface sediments of Qingdao coastal area[J].Environmental Science,2010,31(11):2713-2722.
[13] Cao Y X,Xin M,Wang B D,et al.Spatiotemporal distribution,source,and ecological risk of polycyclic aromatic hydrocarbons (PAHs) in the urbanized semi-enclosed Jiaozhou Bay,China[J].Science of the Total Environment,2020,717:137224.
[14] Deng B,Zhang J,Zhang G,et al.Enhanced anthropogenic heavy metal dispersal from tidal disturbance in the Jiaozhou Bay,North China[J].Environmental Monitoring and Assessment,2010,161(1-4):349-358.
[15] 刘运令，汪亚平，高建华，等.胶州湾铅-210比活度的分布模式及百年尺度的沉积速率[J].海洋学报(中文版),2010,32(1):83-93.Liu L Y,Wang Y P,Gao J H,et al.Specific activity distribution patterns of lead-210 and sediment accumu-lation rates in the Jiaozhou Bay in Shandong Province,China[J].Haiyang Xuebao (Chinese),2010,32(1):83-93.
[16] US EPA.Method 3535A:Solid-Phase Extraction (SPE)[S].Springfield:National Technical Information Service,2007.
[17] Ma M,Feng Z,Guan C,et al.DDT,PAH and PCB in sediments from the intertidal zone of the Bohai Sea and the Yellow Sea[J].Marine Pollution Bulletin,2001,42(2):132-136.
[18] Bossio J P,Harry J,Kinney C A.Application of ultrasonic assisted extraction of chemically diverse organic compounds from soils and sediments[J].Chemosphere,2008,70(5):858-864.
[19] Kalf D F,Crommentuijn T,Vandeplassche E J.Environmental quality objectives for 10 polycyclic aromatic hydrocarbons (PAHs)[J].Ecotoxicology and Environmental Safety,1997,36(1):89-97.
[20] Cao Z G,Liu J L,Luan Y,et al.Distribution and ecosystem risk assessment of polycyclic aromatic hydrocarbons in the Luan River,China[J].Ecotoxicology,2010,19(5):827-837.
[21] Sharp J H,Benner R,Bennett L,et al.Analyses of dissolved organic carbon in seawater:the JGOFS EqPac methods comparison[J].Marine Chemistry,1995,48(2):91-108.
[22] Hedges J I,Stern J H.Carbon and nitrogen determinations of carbonate-containing solids1[J].Limnology and Oceanography,1984,29(3):657-663.
[23] Wu G,Qin R,Luo W.Polycyclic aromatic hydrocarbons (PAHs) in the Bohai Sea:A review of their distribution,sources,and risks[J].Integrated Environmental Assessment and Management,2022,18(6):1705-1721.
[24] Ma J,Hung H,Macdonald R W.The influence of global climate change on the environmental fate of persistent organic pollutants:A review with emphasis on the Northern Hemisphere and the Arctic as a receptor[J].Global and Planetary Change,2016,146:89-108.
[25] Li P,Cao J,Diao X,et al.Spatial distribution,sources and ecological risk assessment of polycyclic aromatic hydrocarbons in surface seawater from Yangpu Bay,China[J].Marine Pollution Bulletin,2015,93(1):53-60.
[26] 王鹏程，杨凌霄，别淑君，等.港口地区大气PM2.5中多环芳烃污染特征及来源分析[J].环境科学，2022,43(9):4458-4466.Wang P C,Yang L X,Bie S J,et al.Pollution characteristics and source analysis of Atmospheric PM2.5 bound polycyclic aromatic hydrocarbons in a port area[J].Environmental Science,2022,43(9):4458-4466.
[27] 孙红文，张闻.疏水性有机污染物在土壤/沉积物中的赋存状态研究[J].环境化学，2011,30(1):231-241.Sun H W,Zhang W.Existing state of hydrophobic organic compounds in soils and sediments[J].Environmental Science,2011,30(1):231-241.
[28] Srinivasa Reddy M,Basha S,Joshi H V,et al.Seasonal distribution and contamination levels of total PHCs,PAHs and heavy metals in coastal waters of the Alang-Sosiya ship scrapping yard,Gulf of Cambay,India[J].Chemosphere,2005,61(11):1587-1593.
[29] 李先国，邓伟，周晓，等.青岛近岸表层海水中PAHs的分布特征及物源初步解析[J].环境科学，2012,33(3):741-745.Li X G,Deng W,Zhou X,et al.Distribution of PAHs in surface seawater of Qingdao coastal area and their preliminary apportionment[J].Environmental Science,2012,33(3):741-745.
[30] Lu J,Li M,Tan J,et al.Distribution,sources,ecological risk and microbial response of polycyclic aromatic hydrocarbons in Qingdao bays,China[J].Environmental Pollution,2023,338:122687.
[31] Mzoughi N,Chouba L.Distribution and partitioning of aliphatic hydrocarbons and polycyclic aromatic hydrocarbons between water,suspended particulate matter,and sediment in harbours of the West coastal of the Gulf of Tunis (Tunisia)[J].Journal of Environmental Monitoring,2011,13(3):689-698.
[32] Tong Y,Chen L,Liu Y,et al.Distribution,sources and ecological risk assessment of PAHs in surface seawater from coastal Bohai Bay,China[J].Marine Pollution Bulletin,2019,142:520-524.
[33] Sinaei M,Mashinchian A.Polycyclic aromatic hydrocarbons in the coastal sea water,the surface sediment and mudskipper Boleophthalmus dussumieri from coastal areas of the Persian Gulf:Source investigation,composition pattern and spatial distribution[J].Journal of Environmental Health Science and Engineering,2014,12(1):59.
[34] Wang H J,Wang A M,Bi N H,et al.Seasonal distribution of suspended sediment in the Bohai Sea,China[J].Continental Shelf Research,2014,90:17-32.
[35] Shi Z,Tao S,Pan B,et al.Partitioning and source diagnostics of polycyclic aromatic hydrocarbons in rivers in Tianjin,China[J].Environmental Pollution,2007,146(2):492-500.
[36] Wu X,Wang Y,Zhang Q,et al.Seasonal variation,air-water exchange,and multivariate source apportionment of polycyclic aromatic hydrocarbons in the coastal area of Dalian,China[J].Environmental Pollution,2019,244:405-413.
[37] 张玉凤，宋永刚，宋伦，等.辽东湾海水颗粒相中多环芳烃分布与来源分析[J].水产科学，2018,37(6):793-799.Zhang Y F,Song Y G,Song L,et al.Distribution and source identification of polycyclic aromatic hydrocarbons of suspended particle-phase from Liaodong Bay[J].Fisheries Science,2018,37(6):793-799.
[38] 杨永亮，麦碧娴，潘静，等.胶州湾表层沉积物中多环芳烃的分布及来源[J].海洋环境科学，2003,22(4):38-43.Yang Y L,Mai B X,Pan J,et al.Distribution and sources of polycyclic aromatic hydrocarbons in sediments of Jiaozhou Bay[J].Marine Environmental Science,2003,22(4):38-43.
[39] Sun C,Zhang J,Ma Q,et al.Polycyclic aromatic hydrocarbons (PAHs) in water and sediment from a river basin:Sediment-water partitioning,source identification and environmental health risk assessment[J].Environmental Geochemistry and Health,2017,39(1):63-74.
[40] Adhikari P L,Maiti K,Overton E B.Vertical fluxes of polycyclic aromatic hydrocarbons in the northern Gulf of Mexico[J].Marine Chemistry,2015,168:60-68.
[41] Han B,Liu A,Wang S,et al.Concentration level,distribution model,source analysis,and ecological risk assessment of polycyclic aromatic hydrocarbons in sediments from laizhou bay,China[J].Marine Pollution Bulletin,2020,150:110690.
[42] Zhang X,Wang T,Gao L,et al.Polychlorinated diphenyl ethers (PCDEs) in surface sediments,suspended particulate matter (SPM) and surface water of Chaohu Lake,China[J].Environmental Pollution,2018,241:441-450.
[43] Maruya K A,Risebrough R W,Horne A J.Partitioning of polynuclear aromatic hydrocarbons between sediments from San Francisco Bay and their porewaters[J].Environmental Science & Technology,1996,30(10):2942-2947.
[44] Luo X,Mai B,Yang Q,et al.Distribution and partition of polycyclic aromatic hydrocarbon in surface water of the Pearl River Estuary,South China[J].Environmental Monitoring and Assessment,2008,145(1):427-436.
[45] Zhang J M,Liu G J,Wang R J,et al.Polycyclic aromatic hydrocarbons in the water-SPM-sediment system from the middle reaches of Huai River,China:Distribution,partitioning,origin tracing and ecological risk assessment[J].Environmental Pollution,2017,230:61-71.
[46] Seth R,Mackay D,Muncke J.Estimating the organic carbon partition coefficient and its variability for hydrophobic chemicals[J].Environmental Science & Technology,1999,33(14):2390-2394.
[47] Accardi-Dey A,Gschwend P M.Reinterpreting literature sorption data considering both absorption into organic carbon and adsorption onto black carbon[J].Environmental Science & Technology,2003,37(1):99-106.
[48] Chen C F,Ju Y R,Su Y C,et al.Distribution,sources,and behavior of PAHs in estuarine water systems exemplified by Salt River,Taiwan[J].Marine Pollution Bulletin,2020,154:111029.
[49] Wang J,Nie Y,Luo X,et al.Occurrence and phase distribution of polycyclic aromatic hydrocarbons in riverine runoff of the Pearl River Delta,China[J].Marine Pollution Bulletin,2008,57(6-12):767-774.
[50] Zhang L,Zhang J,Gong M.Size distributions of hydrocarbons in suspended particles from the Yellow River[J].Applied Geochemistry,2009,24(7):1168-1174.
[51] Yunker M B,Macdonald R W,Vingarzan R,et al.PAHs in the Fraser River basin:A critical appraisal of PAH ratios as indicators of PAH source and composition[J].Organic Geochemistry,2002,33(4):489-515.
[52] Wang Y,Song J,Duan L,et al.Historical reconstructions of sedimentary organic matter sources and phytoplankton evolution in the Jiaozhou Bay based on sterols and carbon isotope[J].Marine Pollution Bulletin,2021,165:112109.
[53] Zhou B,Yuan H,Song J,et al.Source,transformation and degradation of particulate organic matter and its connection to microbial processes in Jiaozhou Bay,North China[J].Estuarine,Coastal and Shelf Science,2021,260:107501.
[54] Bnaru D,Harmelin-Vivien M,Gomoiu M-T,et al.Influence of the Danube River inputs on C and N stable isotope ratios of the Romanian coastal waters and sediment (Black Sea)[J].Marine Pollution Bulletin,2007,54(9):1385-1394.
[55] Qi R,Pan L,Liu T,et al.Source risk,ecological risk,and bioeffect assessment for polycyclic aromatic hydrocarbons (PAHs) in Laizhou Bay and Jiaozhou Bay of Shandong Peninsula,China[J].Environmental Science and Pollution Research,2022,29(37):56705-56726.
[56] Lin K,Wang R,Tan L,et al.Assessing the potential risks,sources and the relationship between the dissolved and particulate polycyclic aromatic hydrocarbons (PAHs) in the typical semi-enclosed bay,Bohai Bay of China[J].Marine Environmental Research,2023,192:106192.
[57] Mundo R,Matsunaka T,Iwai H,et al.Environmental processes and fate of PAHs at a shallow and enclosed bay:West Nanao Bay,Noto Peninsula,Japan[J].Marine Pollution Bulletin,2022,184:114105.
[58] Luo Y,Tong G,Song Q,et al.Impacts of shipyard oil leakage on the PAHs and PCBs occurrence in Xiangshan Bay,China[J].Marine Environmental Research,2023,190:106057.
[59] Ravanbakhsh M,Jaafarzadeh Haghighi Fard N,Ramezani Z,et al.Assessment of polycyclic aromatic hydrocarbons (PAHs) in seawater and sediments,human and ecological risks,Northern Coastline of Persian Gulf[J].Bulletin of Environmental Contamination and Toxicology,2023,110(1):39-48.
[60] Ahmed O E,Mahmoud S A,El Nady M M.Compositions,sources,and ecological risk assessment of polyaromatic hydrocarbons in surface sediments along the Suez Gulf,Egypt[J].Petroleum Science and Technology,2016,34(23):1929-1938.
[61] Zhang A,Zhao S,Wang L,et al.Polycyclic aromatic hydrocarbons (PAHs) in seawater and sediments from the northern Liaodong Bay,China[J].Marine Pollution Bulletin,2016,113(1-2):592-599.
[62] Wu Y,Zhang Z,Huang W,et al.Environmental profile,potential sources,and ecological risk of polycyclic aromatic hydrocarbons in a typical coastal bay and outer bay area[J].Environmental Science and Pollution Research,2023,30(31):77757-77770.
基本信息:
DOI：10.16441/j.cnki.hdxb.20240088
中图分类号:X55;X826
引用信息:
[1]王晓雪,曹亚俐,金红,等.胶州湾不同环境介质中多环芳烃的分布、来源和生态风险评价[J].中国海洋大学学报(自然科学版),2025,55(05):100-112.DOI:10.16441/j.cnki.hdxb.20240088.
基金信息:
崂山实验室“十四五”重大项目：海洋环境新污染物防治与水环境安全项目（LSKJ202203901）; 中央高校基本科研业务费专项（202262009,202464007）资助~~
2024-03-10
2024
2024-04-07
2024-04-09
2024
1
2025-04-28
2025-04-28