沉积环境

基于多参数指标的长江口滨岸多环芳烃来源辨析

展开
  • 1. 华东师范大学资源与环境科学学院, 教育部地理信息科学重点实验室, 上海200062;
    2. 华东师范大学河口海岸学国家重点实验室, 上海200062
欧冬妮(1979-), 女, 福建泉州人, 博士, 主要从事河口生物地球化学研究。E-mail: odn79@yahoo.com.cn

收稿日期: 2007-12-06

  修回日期: 2008-02-26

  网络出版日期: 2008-05-26

基金资助

国家自然科学基金项目(40671171; 40131020); 高等学校博士学科点专项科研基金(20040269014); 上海市博 士后基金项目(07R214120)

Polycyclic Aromatic Hydrocarbons Sources Identification Based on Multiple Indices from the Yangtze Estuarine and Nearby Coastal Areas

Expand
  • 1. Key Laboratory of Geographic Information Science of the Ministry of Education, School of Resources and Environment Science, East China Normal University, Shanghai 200062, China;
    2. State Key Laboratory of Estuarine and Coastal Research, East China Normal University, Shanghai 200062, China

Received date: 2007-12-06

  Revised date: 2008-02-26

  Online published: 2008-05-26

Supported by

National Natural Science Foundation of China, No.40671171; No. 40131020; Doctoral Program of MOE, No.20040269014; Shanghai Postdoctoral Foundation, No.07R214120

摘要

在长江口滨岸及临近排污口、滨岸河流、城市中心城区采集悬浮颗粒物、表层沉积物、街道灰尘等样品, 分别利用GC-MS 和GC-C-IRMS 定量分析了不同环境介质中的多环芳烃 (PAHs) 与有机单体化合物稳定碳同位素(δ13C), 开展了基于PAH 环数、分子量特征比值和有机单体化合物稳定碳同位素组成等参数指标的长江口滨岸悬浮颗粒物与表层沉积物中PAHs 源解析研究。研究结果显示, 长江口滨岸悬浮颗粒物与表层沉积物中的PAH 化合物主要以3~4 环为主, 与吴淞排污口、石洞口污水处理厂、黄浦江、滨岸小河流以及上海中心城区等潜在来源区域不同环境介质中的PAHs 组成特征相似, 主要来源于汽油、柴油、煤炭和木材的不完全燃烧以及石油残余物的混合。其中, 木材和煤炭不完全燃烧形成的PAHs 以及石油残余物, 枯季经过滨岸河流及排污口直接输入, 洪季则为城市街道灰尘被暴雨冲刷, 随地表 径流最终汇入河口; 汽车排放(汽油、柴油不完全燃烧) 产生的PAHs 主要富集在城市交通区和商业区的街道灰尘中, 枯季借助区域盛行风迁移至河口区, 洪季则主要通过暴雨径流冲刷进入河口。

本文引用格式

欧冬妮, 刘敏, 许世远, 程书波, 侯立军, 王丽丽 . 基于多参数指标的长江口滨岸多环芳烃来源辨析[J]. 地理学报, 2008 , 63(5) : 535 -543 . DOI: 10.11821/xb200805009

Abstract

Samples of suspended particulate matters (SPMs), surface sediment and road dusts were collected in the Yangtze estuarine and nearby coastal areas, coastal rivers, and Shanghai metropolitan area, respectively. Sixteen polycyclic aromatic hydrocarbons (PAHs) in the USEPA priority-controlled list were determined by GC-MS and compound-specific stable carbon isotopes of individual PAHs were analyzed by GC-C-IRMS. PAHs sources of SPMs and surface sediments in the Yangtze estuarine and nearby coastal areas were examined using multiple source identification techniques which integrated molecular mass indices with organic compound-specific stable isotopes. The results showed that the third and fourth rings PAH compounds were dominant in SPMs and surface sediments, similar to those in Wusong sewage discharge outlet, Shidongkou sewage disposal plant, Huangpu River, coastal rivers and Shanghai metropolitan area. Principal component analysis (PCA) integrated with molecular mass indices indicated that gasoline, diesel oil, coal and wood combustion and petroleum were the main sources for PAHs in the Yangtze Estuary. Use of PAH compound-specific stable isotopes tracked PAHs input pathways. PAHs derived from wood and coal combustion and petroleum were input into the Yangtze estuarine and nearby coastal areas by coastal rivers, sewage discharge outlets in dry season and urban storm water runoff in flood season. PAHs derived from vehicle emissions were mainly accumulated in road dusts from urban traffic lines and commercial district, which entered the coastal area by the northwest prevailing wind in dry season and storm water runoff in flood season.

参考文献


[1] Baumard P, Budzinski H, Michon Q et al. Origin and bioavailability of PAHs in the Mediterranean Sea from mussel and sediment records. Estuarine, Coastal and Shelf Science, 1998, 47: 77-90.

[2] Oros D R, Ross J R M. Polycyclic aromatic hydrocarbons in San Francisco Estuary sediments. Marine Chemistry, 2004, 86: 169-184.

[3] 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. Organic Geochemistry, 2002, 33: 489-515.

[4] Yim U H, Hong S H, Shim W J et al. Spatio-temporal distribution and characteristics of PAHs in sediments from Masan Bay, Korea. Marine Pollution Bulletin, 2005, 50: 319-326.

[5] Currie L A, Klouda G A, Benner B A et al. Isotopic and molecular marker validation, including direct molecular 'dating' (GC/AMS). Atmospheric Environment, 1999, 33: 2789-2806.

[6] O'Malley V P, Abrajano Jr T A, Hellou J. Stable carbon isotopic apportionment of individual polycyclic aromatic hydrocarbons in St.John's Harbour, Newfoundland. Environmental Science and Technology, 1996, 30: 634-639.

[7] Smirnov A, Abrajano Jr T A, Smirnov A et al. Distribution and sources of PAHs in the sediments of Lake Erie (Part 1), Spatial distribution, transport, and deposition. Organic Geochemistry, 1998, 29: 1813-1828.

[8] Mcrae C, Sun C, Snape C E et al. δ13C values of coal-derived PAHs from different processes and their application to source apportionment. Organic Geochemistry, 1999, 30: 881-889.

[9] Reddy C M, Pearson A, Xu L et al. Radiocarbon as a tool to apportion the sources of polycyclic aromatic hydrocarbons and black carbon in environmental samples. Environmental Science and Technology, 2002, 36: 1774-1782.

[10] Stark A, Abrajano Jr T A, Hellou J et al. Molecular and isotopic characterization of polycyclic aromatic hydrocarbon distribution and sources at the international segment of the St.Lawrence River. Organic Geochemistry, 2003, 34: 225-237.

[11] Walker S E, Dickhut R M, Chisholm-Brause C J et al. Molecular and isotopic identification of PAH sources in a highly industrialized urban estuary. Organic Geochemistry, 2005, 36: 619-632.

[12] Kim M, Kennicutt II M C, Qan Y R. Polycyclic aromatic hydrocarbon purification procedures for compound specific isotope analysis. Environmental Science and Technology, 2005, 39: 670-6776.

[13] Liu Zhengtao, Jiang Fuxin, Wang Wanhua et al. Character analysis of organic pollutants in Yangtze Estuary area. Research of Environmental Sciences, 2006, 19(2): 1-5.
[刘征涛, 姜福欣, 王婉华等. 长江河口区域有机污染物的特 征分析. 环境科学研究, 2006, 19(2): 1-5.]

[14] Liu Min, Xu Shiyuan, Chen Zhenlou. Distribution characteristics of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of tidal flats of the Yangtze Estuary. China Environmental Science, 1998, 18(3): 284-288.
[刘敏, 许世远, 陈 振楼. 上海南汇淤泥质潮滩表层沉积物中多环芳烃. 中国环境科学, 1998, 18(3): 284-288.]

[15] Liu Min, Xu Shiyuan, Yu Lizhong et al. Distribution of polycyclic aromatic hydrocarbons in sediments of Baoshan core in Changjiang Estuary. Marine Environmental Science, 2000, 19(4): 9-12.
[刘敏, 许世远, 俞立中等. 长江口宝山孔 沉积物中多环芳烃的分布. 海洋环境科学, 2000, 19(4): 9-12.]

[16] Ou Dongni, Liu Min, Cheng Shubo et al.. Distribution and ecological risk assessment of polycyclic aromatic hydrocarbons in suspended particulate matters from the Yangtze Estuarine and coastal areas. Resources and Environment in the Yangtze Basin, 2007, 16(5): 623-626.
[欧冬妮, 刘敏, 程书波等. 河口滨岸悬浮颗粒物中多环芳 烃分布与风险评价. 长江流域资源与环境, 2007, 16(5): 620-623.]

[17] Laflamme R E, Hites R A. Geochim. The globe distribution of polycyclic aromatic hydrocarbons in recent sediments. Geochim. Cosmochim. Acta, 1978, 42: 289-303.

[18] Lake J L, Norwood C, Dimock C et al. Origins of polycyclic aromatic hydrocarbons in estuarine sediments. Geochim. Cosmochim. Acta, 1979, 43: 1847-1854.

[19] Yunker M B, Snowdon L R, Macdonald R W et al. Polycyclic Aromatic Hydrocarbon Composition and Potential Sources for Sediment Samples from the Beaufort and Barents Seas. Environmental Science and Technology, 1996, 30: 1310-1320.

[20] Muel B, Saguem S. Determination of 23 polycyclic aromatic hydrocarbons in atmospheric particulate matter of the Paris area and photolysis by sun light. International Journal Environmental Analytical Chemistry, 1985, 19: 111-131.

[21] Tolosa J, Bayona J M, Albaige's J. Aliphatic and polycyclic aromatic hydrocarbons and sulfur/oxygen derivatives in northwestern Mediterranean sediments: Spatial and temporal variability, fluxes, and budgets. Environmental Science and Technology, 1996, 30: 2495-2503.

[22] Mai B X, Qi S H, Zeng E Y et al. Distribution of polycyclic aromatic hydrocarbons in the coastal region of Macao, China: Assessment of input sources and transport pathways using compositional analysis. Environmental Science and Technology, 2003, 37: 4855-4863.

[23] Takada H, Onda T, Ogura N. Determination of polycyclic aromatic hydrocarbons in urban street dusts and their source materials by capillary gas chromatography. Environmental Science and Technology, 1990, 24: 1179-1186.

[24] Wise S A, Benner B A, Byrd G D et al. Determination of polycyclic aromatic hydrocarbons in a coal tar standard reference material. Anal. Chem., 1988, 60: 887-894.

[25] Grimmer G, Jacob J, Naujack K W et al. Profile of the polycyclic aromatic hydrocarbons from used engine oil-inventory by GCGC/MS-PAH in environmental materials (Part 2). Fresenius A. Anal. Chem., 1981, 309: 13-19.

[26] Budzinski H, Jones I, Bellocq J, Pie'rard C et al. Evaluation of sediment contamination by polycyclic aromatic hydrocarbons in the Gironde estuary. Marine Chemistry, 1997, 58: 85-97.

[27] O'Malley V P, Abrajano Jr T A, Hellou J. Determination of the 13C/12C ratios of individual PAH from environmental samples, can PAH sources be apportioned? Organic Geochemistry, 1994, 21: 809-822.

[28] Glaser B, Dreyer A, Bock M et al. Source apportionment of organic pollutants of a Highway-Traffic-Influenced urban area in Bayreuth (Germany) using biomarker and stable carbon isotope signatures. Environmental Science and Technology, 2005, 39: 3911-3917.

[29] O'Malley V P, Burke R A, Schlotzhauer W S. Using GC-MS/Combustion/IRMS to determine the 13C//12C ratios of individual hydrocarbons produced from the combustion of biomass materials-application to biomass burning. Organic Geochemistry, 1997, 27: 567-581.

文章导航

/