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多环芳烃(Polycyclic aromatic hydrocarbons, PAHs)作为一类具有“三致”效应的持久性有机污染物,在高强度人类活动的近海地区广泛分布,环境风险备受关注。目前,由于缺乏对入海排污单元和重点行业PAHs排放量时空变化的认知,对PAHs污染陆海统筹防治形成制约。本研究环胶州湾排污单元为研究区域,分析了其2022年8月(丰水期)和2023年4月(枯水期)7条入湾河流和4个公共污水处理厂直排口水体中溶解态PAHs(Dissolved polycyclic aromatic hydrocarbons, DPAHs)和颗粒态PAHs(Particulate polycyclic aromatic hydrocarbons, PPAHs)的组成、浓度及入海通量的时空变化,应用特征比值和主成分分析法(Principal component analysis-multiple linear regression, PCA-MLR),解析环湾地区PAHs的主要来源,采用排放因子法,估算了胶州湾排污单元PAHs的排放量及主要行业贡献率。丰水期和枯水期,入胶州河流和直排口水体中DPAHs浓度,受光降解等环境因素的影响,整体呈现丰水期低于枯水期的特征,均值分别为(207.4±52.9)和(645.9±184.8) ng·L-1;PPAHs浓度受颗粒物通量增加和吸附效应增强的协同作用,整体则呈现丰水期高于枯水期的特征,均值分别为(78.3±132.3)和(17.7±11.1)μg·g-1;其中,丰水期DPAHs以3环为主,枯水期以4环为主;丰水期和枯水期PPAHs均以3环为主。丰水期PAHs的入海通量为1 645.5 kg·month-1,约为枯水期的13.6倍。基于PAHs特征比值和PCA-MLR结果表明,环湾排污单元PAHs主要来源于石油煤炭和生物质不完全燃烧过程。环湾排污单元内16种PAHs的年排放量为82.37 t·a-1,按照占比,排污单元由高到低依次为大沽河(45.8%)、墨水河(20.3%)、海泊河(10.8%)、李村河(7.0%)、娄山河(5.7%)、镰湾河(4.1%)、团岛(3.5%)和洋河(2.8%)排污单元。按照重点行业贡献率,由高到低依次为交通源(51.7%)、生活源(32.3%)和工业源(16.1%)。研究结果可为胶州湾PAHs污染精准施策提供科学依据。
Abstract:PolycyclicAromaticHydrocarbons(PAHs), as a kind of persistent organic pollutants with "three-cause" effect, are widely distributed in the offshore areas with high intensity of human activities, and their environmental risks have attracted much attention. At present, due to the lack of understanding of the spatial and temporal changes of PAHs emissions from offshore sewage units and key industries, the systemic prevention and control of PAHs pollution in the Gulf is restricted. In this study, the pollutant discharging unit(PDU) unit around Jiaozhou Bay(JZB) was taken as the research area, and the composition, concentration and temporal and spatial changes of dissolved PAHs(DPAHs) and particulate PAHs(PPAHs) in the water bodies of seven rivers entering the bay and four public sewage treatment plants in the August, 2022(wet season) and the April, 2023(dry season) were analyzed. The main sources of PAHs in the ring area were analyzed using the characteristic ratio and principal component analysis(PCA-MLR) method, and the emission factor method was used to estimate the emission of PAHs in the JZB PDU and the contribution rate of major industries. During the wet season and dry season, the concentration of DPAHs in the rivers entering JZB and the direct discharge water is affected by environmental factors such as photodegradation, and the overall characteristics are lower in the wet season than in the dry season, with the average values of(207.4±52.9) and(645.9±184.8) ng·L-1; respectively. The concentration of PPAHs was influenced by the increase of particle flux and the enhancement of adsorption effect, and it was higher in wet season than in dry season, with average values of(78.3±132.3) and(17.7±11.1) μg·g-1, respectively. Among them, DPAHs is mainly composed of 3 rings in wet season and 4 rings in dry season; In wet season and dry season, PPAHs is mainly composed of 3 rings. The flux of PAHs into the sea in wet season is 1 645.5 kg·month-1, which is about 13.6 times that in dry season. Based on the analysis of PAHs characteristic ratio and PCA-MLR results show that PAHs in the sewage disposal unit around the bay mainly come from the incomplete combustion process of petroleum, coal and biomass. The annual emission of 16 kinds of PAHs in the sewage units around JZB is 82.37 t·a-1, and PDUs in descending order are Dagu River(45.8%), Moshui River(20.3%), Haibo River(10.8%), Licun River(7.0%), Loushan River(5.7%), Lianwan River(4.1%), Tuandao River(3.5%) and Yang River(2.8%). According to the contribution rate of key industries, from high to low, it is traffic source(51.7%), life source(32.3%) and industrial source(16.1%). The research results can provide scientific basis for the precise policy of PAHs pollution in Jiaozhou Bay.
[1] Chen B L,Xuan X D,Zhu L Z,et al.Distributions of polycyclic aromatic hydrocarbons in surface waters,sediments and soils of Hangzhou City,China[J].Water Research,2004,38(16):3558-3568.
[2] Ce Y,Zhong N N,Chen D Y,et al.Distribution characteristics of polycyclic aromatic hydrocarbons(PAHs) in suspended particulate matter of surface water in coal-mining area,China[J].China Environmental Science,2007,27(4):488-492.
[3] Lee C C,Chen C S,Wang Z X,et al.Polycyclic aromatic hydrocarbons in 30 river ecosystems,Taiwan:Sources,and ecological and human health risks[J].Science of the Total Environment,2021,795:148867.
[4] X L,Zhang G,Jones K C,et al.Compositional fractionation of polycyclic aromatic hydrocarbons (PAHs) in mosses (WILS.) from the northern slope of Nanling Mountains,South China[J].Atmospheric Environment,2005,39(30):5490-5499.
[5] US EPA.Method 3535A:Solid-Phase Extration (SPE)[S].Springfield:National Technical Information Service,2007.
[6] 孟令辰,姚雯芮,付晓丽,等.入海河流中典型新污染物的分布特征及其生态风险——以天津市为例[J].海洋环境科学,2024,43:865-871.Meng L C,Yao W R,Fu X L,et al.Distribution characteristics and ecological risks of emerging contaminants in rivers discharging to sea:A case study of Tianjin[J].Marine Environmental Science,2024,43:865-871.
[7] Wang M,Wang C,Li Y.Petroleum hydrocarbons in a water-sediment system from Yellow River estuary and adjacent coastal area,China:Distribution pattern,risk assessment and sources[J].Marine Pollution Bulletin,2017,122(1-2):139-148.
[8] 褚春莹,但丽霞,蒋海威,等.胶州湾入海河流和排污口水体中壬基酚的污染状况调查及入海通量核算[J].中国环境监测,2013,29:29-33.Chu C Y,Dan L X,Jiang H W,et al.Investigation of nonylphenol pollution and estimation of flux into the sea in rivers and outfalls discharging into Jiaozhou Bay[J].Environmental Monitoring in China,2013,29:29-33.
[9] 李姗姗,于晓霞,张鹏,等.胶州湾入海源区氮磷超载状况分析[J].环境科学与技术,2021,44:11-18.Li S S,Yu X X,Zhang P,et al.Analysis of nitrogen and phosphorus overloading in source inputs to Jiaozhou Bay[J].Environmental Science & Technology,2021,44:11-18.
[10] Han B,Liu A,Gong J W,et al.Spatial distribution,source analysis,and ecological risk assessment of polycyclic aromatic hydrocarbons (PAHs) in the sediments from rivers emptying into Jiaozhou Bay,China[J].Marine Pollution Bulletin,2021,168:112394.
[11] 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.
[12] Han B,Liu A,He S,et al.Composition,content,source,and risk assessment of PAHs in intertidal sediment in Shilaoren Bay,Qingdao,China[J].Marine Pollution Bulletin,2020,159:111499.
[13] Lu J X,Li M T,Tan J C,et al.Distribution,sources,ecological risk and microbial response of polycyclic aromatic hydrocarbons in Qingdao bays,China[J].Environmental Pollution,2023,338:122687.
[14] 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.
[15] 关小敏,曾光明,陈耀宁,等.水体沉积物多环芳烃源解析技术研究进展[J].安全与环境学报,2010,10:85-89.Guan X M,Zeng G M,Chen Y N,et al.Research progress on source apportionment techniques for polycyclic aromatic hydrocarbons (PAHs) in aquatic sediments[J].Journal of Safety and Environment,2010,10:85-89.
[16] Shen H Z,Huang Y,Wang R,et al.Global atmospheric emissions of polycyclic aromatic hydrocarbons from 1960 to 2008 and future predictions[J].Environmental Science & Technology,2013,47,(12):6415-6424.
[17] 乔旭东.胶州湾排污管理区及其主要排海化学污染物分配容量的准确计算研究[D].青岛:中国海洋大学,2009.Qiao X D.The study on Jiaozhou Bay Discharge Regionsand Accurate Calculations of Their Allocated Capacities of Major Pollutants[D].Qingdao:Ocean University of China,2009.
[18] 王瑶瑶,李俊龙,李凤超,等.胶州湾入海河流和排污口全氟多氟化合物的污染状况及来源解析[J].中国海洋大学学报(自然科学版),2025,55(3):55-69.Wang Y Y,Li J L,Li F C.et al.Pollution status and source analysis of per- and polyfluoroalkyl substances in rivers and sewage outlets of Jiaozhou Bay[J].Periodical of Ocean University of China,2024,54(3):55-69.
[19] GB50179—2015.河流流量测验规范[S].2016.GB50179—2015.Specification for River Flow Test[S].2016.
[20] 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.
[21] 山东省统计局.2023年山东省统计年鉴[DS/OL].中国统计出版社,(2023)[2023-12-28].http://tjj.shandong.gov.cn/tjnj/nj2023/zk/indexch.htm.Shandong Provincial Bureau of Statistics.Statistical Yearbook of Shandong Province in 2023 [DS/OL].China Statistics Publishing House,(2023)[2023-12-28].http://tjj.shandong.gov.cn/tjnj/nj2023/zk/indexch.htm.
[22] 青岛市统计局.2023年青岛市统计年鉴[DS/OL].中国统计出版社,(2023)[2023-10-26].http://qdtj.qingdao.gov.cn/tongjisj/tjsj_tjnj/tjnj_2023/202310/t20231026_7560532.shtml.Qingdao Municipal Bureau of Statistics.Statistical Yearbook of Qingdao in 2023 [DS/OL].China Statistics Publishing House,(2023)[2023-10-26].http://qdtj.qingdao.gov.cn/tongjisj/tjsj_tjnj/tjnj_2023/202310/t20231026_7560532.shtml.
[23] 青岛市第二次污染源普查领导小组办公室.青岛市污染源普查技术报告(2017年)[R].青岛:青岛市环境保护局,2018.Qingdao Leading Group Office for the Second Pollution Source Survey.Qingdao Pollution Source Survey Technical Report (2017)[R].Qingdao:Qingdao Environmental Protection Bureau,2018.
[24] 刘伟亚,刘敏,杨毅,等.上海市多环芳烃排放清单构建及排放趋势预测[J].长江流域资源与环境,2015,24:1003-1011.Liu W Y,Liu M,Yang Y,et al.Development of polycyclic aromatic hydrocarbons (PAHs) emission inventory and projection of emission trends in Shanghai[J].Resources and Environment in the Yangtze Basin,2015,24:1003-1011.
[25] Zhang P,Zhou Y,Chen Y,et al.Construction of an atmospheric PAH emission inventory and health risk assessment in Jiangsu,China[J].Air Quality Atmosphere and Health,2023,16(3):629-640.
[26] 李莉,梁生康,石晓勇,等.2007年环胶州湾入海河流污染状况和污染物入海通量分析[J].环境科学与管理,2009,34:23-28.Li L,Liang S K,Shi X Y,et al.Pollution status and flux estimation of land-based pollutants discharging into Jiaozhou Bay via Surrounding Rivers (2007)[J].Environmental Science and Management,2009,34:23-28.
[27] 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.
[28] Chen C T,Lin T,Sun X,et al.Spatiotemporal distribution and particle-water partitioning of polycyclic aromatic hydrocarbons in Bohai Sea,China[J].Water Research,2023,244:120440.
[29] 刘洁,郭占荣,袁晓婕,等.胶州湾周边河流溶解态营养盐的时空变化及入海通量[J].环境化学,2014,33:262-268.Liu J,Guo Z R,Yuan X J,et al.Spatiotemporal variations and fluxes of dissolved nutrients from rivers surrounding Jiaozhou Bay[J].Environmental Chemistry,2014,33:262-268.
[30] He X P,Chen J H,Li X T,et al.Pollution status,influencing factors and environmental risks of neonicotinoids,fipronil and its metabolites in a typical semi-closed bay in China[J].Environmental Pollution,2021,291:118210.
[31] 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.
[32] Ji G C,Zou L,Guan W C,et al.Partition,transportation and ecological risks of polycyclic aromatic hydrocarbons (PAHs) under heavy anthropogenic estuary:A case study in the Xiaoqing River Estuary,North China[J].Regional Studies in Marine Science,2021,43:101604.
[33] Shi Z,Tao S,Pan B,et al.Contamination of rivers in Tianjin,China by polycyclic aromatic hydrocarbons[J].Environmental Pollution,2005,134(1):97-111.
[34] Montuori P,Aurino S,Garzonio F,et al.Distribution,sources and ecological risk assessment of polycyclic aromatic hydrocarbons in water and sediments from Tiber River and estuary,Italy[J].Science of the Total Environment,2016,566:1254-1267.
[35] Zhang Z L,Huang J,Yu G,et al.Occurrence of PAHs,PCBs and organochlorine pesticides in the Tonghui River of Beijing,China[J].Environmental Pollution,2004,130(2):249-261.
[36] Guo W,He M C,Yang Z F,et al.Distribution of polycyclic aromatic hydrocarbons in water,suspended particulate matter and sediment from Daliao River watershed,China[J].Chemosphere,2007,68(1):93-104.
[37] 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.
[38] Li G C,Xia X H,Yang Z F,et al.Distribution and sources of polycyclic aromatic hydrocarbons in the middle and lower reaches of the Yellow River,China[J].Environmental Pollution,2006,144(3):985-993.
[39] Lv J,Xu J,Guo C,et al.Spatial and temporal distribution of polycyclic aromatic hydrocarbons (PAHs) in surface water from Liaohe River Basin,northeast China[J].Environmental Science and Pollution Research,2014,21(11):7088-7096.
[40] Sun J H,Wang G L,Chai Y,et al.Distribution of polycyclic aromatic hydrocarbons (PAHs) in henan reach of the Yellow River,Middle China[J].Ecotoxicology and Environmental Safety,2009,72(5):1614-1624.
[41] Countway R E,Dickhut R M,Canuel E A.Polycyclic aromatic hydrocarbon (PAH) distributions and associations with organic matter in surface waters of the York River,VA Estuary[J].Organic Geochemistry,2003,34(2):209-224.
[42] Mitra S,Bianchi T S.A preliminary assessment of polycyclic aromatic hydrocarbon distributions in the lower Mississippi River and Gulf of Mexico[J].Marine Chemistry,2003,82(3-4):273-288.
[43] Marr L C,Kirchstetter T W,Harley R A,et al.Characterization of polycyclic aromatic hydrocarbons in motor vehicle fuels and exhaust emissions[J].Environmental Science & Technology,1999,33(18):3091-3099.
[44] Yang W,Lang Y H,Bai J,et al.Quantitative evaluation of carcinogenic and non-carcinogenic potential for PAHs in coastal wetland soils of China[J].Ecological Engineering,2015,74:117-124.
[45] Khalili N R,Scheff P A,Holsen T M.Pah source fingerprints for coke ovens,diesel and gasoline-engines,highway tunnels,and wood combustion emissions[J].Atmospheric Environment,1995,29(4):533-542.
[46] Li J,Li F D.Polycyclic aromatic hydrocarbons in the Yellow River estuary:Levels,sources and toxic potency assessment[J].Marine Pollution Bulletin,2017,116(1-2):479-487.
[47] Hildemann L M,Markowski G R,Cass G R.Chemical-composition of emissions from urban sources of fine organic aerosol[J].Environmental Science & Technology,1991,25(4):744-759.
[48] 穆玺龙.中国多环芳烃排放清单 [D].北京:中国石油大学,2016.Mu X L.An Emission Inventory of Polycyclic Aromatic Hydrocarbons in China[D].Beijing:China University of Petroleum,2016.
[49] 高佳佳,罗维,奚晓霞.首都水源地——洋河流域人为源多环芳烃(PAHs)排放清单估算及其影响分析[J].环境科学,2014,35:4573-4581.Gao J J,Luo W,Xi X X.Emission inventory estimation and impact analysis of anthropogenic polycyclic aromatic hydrocarbons (PAHs) in the Yang River Basin - a critical water source for the capital region[J].Environmental Science,2014,35:4573-4581.
[50] 蒋秋静,李跃宇,胡新新,等.太原市多环芳烃(PAHs)排放清单与分布特征分析[J].中国环境科学,2013,33:14-20.Jiang Q J,Li Y Y,Hu X X,et al.Emission inventory and distribution characteristics of polycyclic aromatic hydrocarbons (PAHs) in Taiyuan City[J].China Environmental Science,2013,33:14-20.
基本信息:
DOI:10.16441/j.cnki.hdxb.20250162
中图分类号:X55;X522
引用信息:
[1]闫一丹,王晓雪,梁生康,等.胶州湾入海河流及直排污口水体中多环芳烃污染特征及来源解析[J].中国海洋大学学报(自然科学版),2026,56(05):71-85.DOI:10.16441/j.cnki.hdxb.20250162.
基金信息:
崂山实验室科技创新项目(LSKJ202203901); 山东省重点研究发展项目(2022QNLM040002); 中央高校基本科研业务费专项(20247200)资助~~
2025-05-12
2025
2025-06-22
2025-06-25
2025
1
2026-04-27
2026-04-27