沉积物中PAHs不可萃取组分及其对源解析的影响

韩尔瑄; 李小水; 秦世斌; 刘威杰; 李欢; 叶子杨; 祁士华

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (7) : 3916-3924.

环境生态

沉积物中PAHs不可萃取组分及其对源解析的影响

韩尔瑄¹, 李小水¹, 秦世斌², 刘威杰³, 李欢³, 叶子杨¹, 祁士华^1,3

作者信息 +

Study on non-extractable residues of PAHs in sediments and their effects on source analysis.

HAN Er-xuan¹, LI Xiao-shui¹, QIN Shi-bin², LIU Wei-jie³, LI Huan³, YE Zi-yang¹, QI Shi-hua^1,3

Author information +

文章历史 +

摘要

以洞庭湖表层沉积物为研究对象,通过硅烷化与酸化组合法分析了样品中多环芳烃(PAHs)的不可萃取组分浓度,探究其对PAHs污染及来源解析研究的影响.结果表明,PAHs不可萃取组分的引入显著改变了样品中PAHs的浓度和组成特征,使3环PAHs的占比由可萃取组分中的(19.78%±8.80%)升高到总浓度中的(32.97%±11.16%).PAHs不可萃取组分占比与有机碳和粒度未呈现显著强相关性,更多是受目标物总浓度和污染来源的影响.来源解析表明,考虑不可萃取组分后,主要污染来源由交通排放源(46.91%)转变为生物质和煤炭燃烧源(40.70%).不可萃取组分对PAHs来源解析具有重要作用.

Abstract

Surface sediments of Dongting Lake were selected as the research object and the concentrations of non-extractable polycyclic aromatic hydrocarbons (PAHs) in the samples were analyzed using a combination of silanization and acidification methods. The study aims to investigate the impact of non-extractable residues on the pollution levels and source analysis of PAHs. The inclusion of non-extractable residues significantly altered the concentration and compositional characteristics of PAHs in the samples, raising the proportions of 3-ring PAHs from (19.78% ± 8.80%) in extractable fractions to (32.97% ± 11.16%) in total concentrations. The proportions of non-extractable PAHs did not exhibit a significant strong correlation with organic carbon or particle size, but were more affected by the total concentration of targets and pollution sources. Source apportionment results revealed that, after considering non-extractable residues, the main pollution sources shifted from traffic emissions (46.91%) to biomass and coal combustion sources (40.70%). The non-extractable residues play an important role in the source analysis of PAHs.

导出引用

韩尔瑄, 李小水, 秦世斌, 刘威杰, 李欢, 叶子杨, 祁士华. 沉积物中PAHs不可萃取组分及其对源解析的影响[J]. 中国环境科学. 2025, 45(7): 3916-3924

HAN Er-xuan, LI Xiao-shui, QIN Shi-bin, LIU Wei-jie, LI Huan, YE Zi-yang, QI Shi-hua. Study on non-extractable residues of PAHs in sediments and their effects on source analysis.[J]. China Environmental Science. 2025, 45(7): 3916-3924

中图分类号： X132

参考文献

[1] Meng Y, Liu X, Lu S, et al. A review on occurrence and risk of polycyclic aromatic hydrocarbons (PAHs) in lakes of China [J]. Science of The Total Environment, 2019,651:2497-2506.
[2] Dat N D, Chang M B. Review on characteristics of PAHs in atmosphere, anthropogenic sources and control technologies [J]. Science of the Total Environment, 2017,609:682-693.
[3] Han J, Liang Y, Zhao B, et al. Polycyclic aromatic hydrocarbon (PAHs) geographical distribution in China and their source, risk assessment analysis [J]. Environmental Pollution, 2019,251:312-327.
[4] 温佳乐,李岩,李晔,等.太湖表层沉积物多环芳烃的空间分布、来源及其风险 [J]. 湖泊科学, 2024,36(4):1082-1097. Wen J L, Li Y, Li Y, et al. The spatial distribution,source and risk of polycyclic aromatic hydrocarbon in surface sediments of Lake Taihu [J]. Journal of Lake Science, 2024,36(4):1082-1097.
[5] 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.
[6] Qian Y, Zheng H, Ouyang X, et al. Distinct anthropogenic signatures: A comparative analysis of polycyclic aromatic hydrocarbons in sediments from two southeastern Chinese bays [J]. Marine Pollution Bulletin, 2024,203:116489.
[7] Chen Y F, Kao C L, Yang J F, et al. A Simple extraction method for determination of high molecular weight polycyclic aromatic hydrocarbons in sediments by gas chromatography–mass spectrometry [J]. Journal of the Chinese Chemical Society, 2015,62(9):766-771.
[8] Santos M D, Cerqueira M R, De Oliveira M A, et al. Box–Behnken design applied to ultrasound-assisted extraction for the determination of polycyclic aromatic hydrocarbons in river sediments by gas chromatography/mass spectrometry [J]. Analytical Methods, 2014,6(6): 1650-1656.
[9] Choi M, Kim Y J, Lee I S, et al. Development of a one-step integrated pressurized liquid extraction and cleanup method for determining polycyclic aromatic hydrocarbons in marine sediments [J]. Journal of Chromatography A, 2014,1340:8-14.
[10] He L, Song J. Characterization of extractable and non-extractable polycyclic aromatic hydrocarbons in soils and sediments from the Pearl River Delta, China [J]. Environmental Pollution, 2008,156(3): 769-774.
[11] Schäffer A, Kästner M, Trapp S. A unified approach for including non-extractable residues (NER) of chemicals and pesticides in the assessment of persistence [J]. Environmental Sciences Europe, 2018, 30:1-14.
[12] 丁洋,张原,黄焕芳,等.土壤中持久性有机污染物不可提取态残留的测试方法、生成特征与环境风险研究进展 [J]. 环境化学, 2023,42(1):199-212. Ding Y, Zhang Y, Huang H F, et al. Determination, formation, and environmental risk of non-extractable residue (NER) of persistent organic pollutants (POPs) in soil: A review [J]. Environmental Chemistry, 2023,42(1):199-212.
[13] Qin S B, Li X S, Han E X, et al. Strategies and mechanisms for improving the detection accuracy of nonextractable residues of polycyclic aromatic hydrocarbons in soils [J]. Science of The Total Environment, 2024,943:173908.
[14] Li J, Chang R, Ban X, et al. Aged polycyclic aromatic hydrocarbons as stratigraphic marker in the anthropocene: evidence from Tibetan Lake sediments [J]. Water Research, 2023,245:120652.
[15] Guo J Y, Chen J A, Wang J F, et al. Bound PAHs in sediment and related environmental significance [J]. Archives of Environmental Contamination and Toxicology, 2017,72:530-539.
[16] 万宏滨,周娟,罗端,等.长江中游湖泊表层沉积物多环芳烃的分布、来源特征及其生态风险评价 [J]. 湖泊科学, 2020,32(6):1632-1645. Wan H B, Zhou J, Luo D, et al. Distribution, source characteristics and ecological risk assessment of polycyclic aromatic hydrocarbons in surface sediments of lakes along the middle reaches of the Yangtze River [J]. Journal of Lake Science, 2020,32(6):1632-1645.
[17] Tian H R, Zhang X T, Zhao L L, et al. Variations in the concentration, inventory, source, and ecological risk of polycyclic aromatic hydrocarbons in sediments of the Lake Chaohu [J]. Marine Pollution Bulletin, 2024,201:116188.
[18] 张科.呼伦湖和查干湖沉积物多环芳烃污染历史与来源分析 [D]. 哈尔滨:哈尔滨师范大学, 2019. Zhang K. Pollution history and source analysis of polycyclic aromatic hydrocarbons in sediments of Hulun Lake and Chagan Lake [D]. Harbin: Harbin Normal University, 2019.
[19] 胡昕怡,高冰丽,陈坦,等.截污调水后滇池表层沉积物中16种PAHs的分布特征 [J]. 环境科学, 2019,40(8):3501-3508. Hu X Y, Gao B L, Chen T, et al. Distribution of 16polycyclic aromatic hydrocarbons in Dianchi Lake surface sediments after the integrated water environment control project [J]. Environmental Science, 2019,40(8):3501-3508.
[20] Huang L, Chernyak S M, Batterman S A. PAHs (polycyclic aromatic hydrocarbons), nitro-PAHs, and hopane and sterane biomarkers in sediments of southern Lake Michigan, USA [J]. Science of the Total Environment, 2014,487:173-186.
[21] Yuan H Z, Zhang E L, Lin Q, et al. Sources appointment and ecological risk assessment of polycyclic aromatic hydrocarbons (PAHs) in sediments of Erhai Lake, a low-latitude and high-altitude lake in southwest China [J]. Environmental Science and Pollution Research, 2016,23:4430-4441.
[22] Cao Y, Lin C, Zhang X, et al. Distribution, source, and ecological risks of polycyclic aromatic hydrocarbons in Lake Qinghai, China [J]. Environmental Pollution, 2020,266:115401.
[23] 宋世杰,黄韬,周胜,等.博斯腾湖流域沉积物中多环芳烃的时空分布、来源及生态风险评价 [J]. 环境科学学报, 2019,39(8):2780-2790. Song S J, Huang T, Zhou S et al. Spatial and temporal distribution, sources, and ecological risk assessment of polycyclic aromatic hydrocarbons in sediments of the Bosten Lake watershed [J]. Acta Scientiae Circumstantiae, 2019,39(8):2780-2790.
[24] Tao Y, Xue B, Feng M. Spatial and historical occurrence, sources, and potential toxicological risk of polycyclic aromatic hydrocarbons in sediments of the largest Chinese deep lake [J]. Archives of Environmental Contamination and Toxicology, 2019,77:501-513.
[25] Yang R, Xie T, Li A, et al. Sedimentary records of polycyclic aromatic hydrocarbons (PAHs) in remote lakes across the Tibetan Plateau [J]. Environmental Pollution, 2016,214:1-7.
[26] 杨海君,张海涛,刘亚宾,等.洞庭湖沉积物中持久性有机有毒物质的分布、评价与源解析 [J]. 中国环境科学, 2017,37(4):1530-1539. Yang H J, Zhang H T, Liu Y B, et al. Distribution, assessment and sources analysis of persistent organic toxic chemicals in sediments of Dongting Lake [J]. China Environmental Science, 2017,37(4):1530-1539.
[27] Baumard P, Budzinski H, Garrigues P. Polycyclic aromatic hydrocarbons in sediments and mussels of the western Mediterranean Sea [J]. Environmental Toxicology and Chemistry: An International Journal, 1998,17(5):765-776.
[28] 康杰,胡健,朱兆洲,等.太湖及周边河流表层沉积物中PAHs的分布、来源与风险评价 [J]. 中国环境科学, 2017,37(3):1162-1170. Kang J, Hu J, Zhu Z Z, et al. Distribution, source and risk assessment of PAHs in surface sediments from Taihu Lake and its surrounding rivers [J]. China Environmental Science, 2017,37(3):1162-1170.
[29] Macleod C J, Semple K T. Sequential extraction of low concentrations of pyrene and formation of non-extractable residues in sterile and non-sterile soils [J]. Soil Biology and Biochemistry, 2003,35(11): 1443-1450.
[30] Umeh A C, Duan L, Naidu R, et al. Comparison of single-and sequential-solvent extractions of total extractable benzo [a] pyrene fractions in contrasting soils [J]. Analytical chemistry, 2018,90(19): 11703-11709.
[31] Farrell J, Grassian D, Jones M. Investigation of mechanisms contributing to slow desorption of hydrophobic organic compounds from mineral solids [J]. Environmental Science & Technology, 1999, 33(8):1237-1243.
[32] Cheng H, Hu E, Hu Y. Impact of mineral micropores on transport and fate of organic contaminants: A review [J]. Journal of Contaminant Hydrology, 2012,129:80-90.
[33] Sun L, Zang S. Relationship between polycyclic aromatic hydrocarbons (PAHs) and particle size in dated core sediments in Lake Lianhuan, Northeast China [J]. Science of the Total Environment, 2013,461:180-187.
[34] Thorsen W A, Cope W G, Shea D. Bioavailability of PAHs: Effects of soot carbon and PAH source [J]. Environmental Science & Technology, 2004,38(7):2029-2037.
[35] Zheng H, Qu C, Zhang J, et al. Polycyclic aromatic hydrocarbons (PAHs) in agricultural soils from Ningde, China: levels, sources, and human health risk assessment [J]. Environmental Geochemistry and Health, 2019,41:907-919.
[36] Yu W, Liu R, Wang J, et al. Source apportionment of PAHs in surface sediments using positive matrix factorization combined with GIS for the estuarine area of the Yangtze River, China [J]. Chemosphere, 2015, 134:263-271.
[37] Zhou S, Wang X, Yang Y, et al. Distribution and source identification of polycyclic aromatic hydrocarbons (PAHs) with PCA-MLR and PMF methods in the topsoil of Chengdu at SW, China [J]. Science of The Total Environment, 2024,908:168263.
[38] Simcik M F, Eisenreich S J, Lioy P J. Source apportionment and source/sink relationships of PAHs in the coastal atmosphere of Chicago and Lake Michigan [J]. Atmospheric Environment, 1999,33 (30):5071-5079.
[39] Deng X, Mao L, Peng M, et al. Polycyclic aromatic hydrocarbons in coastal rivers in Jiangsu Province, China: Spatial distribution, source apportionment and human impacts [J]. Journal of Hazardous Materials, 2024,466:133576.
[40] Nielsen T. Traffic contribution of polycyclic aromatic hydrocarbons in the center of a large city [J]. Atmospheric Environment, 1996,30(20): 3481-3490.
[41] Aghadadashi V, Mehdinia A, Bakhtiari A R, et al. Source, spatial distribution, and toxicity potential of polycyclic aromatic hydrocarbons in sediments from Iran's environmentally hot zones, the Persian Gulf [J]. Ecotoxicology and Environmental Safety, 2019,173: 514-525.
[42] Biache C, Mansuy-Huault L, Faure P. Impact of oxidation and biodegradation on the most commonly used polycyclic aromatic hydrocarbon (PAH) diagnostic ratios: Implications for the source identifications [J]. Journal of Hazardous Materials, 2014,267:31-39.