Pollution characteristics and toxicity assessment of PAHs in coal gangue from mine aera in Huaibei
CHEN Xue1,2, XU Dan-dan1, QIAN Ya-hu1, HONG Xiu-ping3, LIANG Han-dong1,2
1. State Key Laboratory of Coal Resources and Safe Mining, China University of Mining and Technology, Beijing 100083, China; 2. College of Geoscience and Surveying Engineering, China University of Mining and Technology, Beijing 100083, China; 3. College of Life Sciences, Huaibei Normal University, Huaibei 235000, China
Abstract:In this paper, we collected 13 gangue samples (7 fresh samples and 6 weathered samples) from Liuqiao Mine in Huaibei, and 16 parent polycyclic aromatic hydrocarbons (16 PAHs) and alkyl-polycyclic aromatic hydrocarbons (a-PAHs) were analyzed by GC-MS/MS on qualitative and quantitative. The results showed that 16PAHs and a-PAHs were generally contained in coal gangue, and the content level of a-PAHs (∑a-PAHs average 587.88ng/g, n=13) was generally higher than that of 16PAHs (∑16PAHs average 505.23ng/g, n=13). The most abundant substance was naphthalene, phenanthrene and chrysene, accounted for 15%, 33% and 15% of ∑16PAHs, respectively. Alkyl-naphthalene and alkyl-phenanthrene in the content of the advantage, accounted for 22% and 40% of ∑a-PAHs. The contents of ∑16PAHs and ∑a-PAHs in the weathered samples was higher than those in the fresh samples. Only the contents of Benzoapyrene and C2-phenanthrene decreased after weathering, and the corresponding contents of C1-Benzoapyrene and phenanthrene increased after weathering. The characteristic ratio shown that the coal gangue samples satisfy 0<C0/(C0+C1-C4) PHE<0.25 and 0.2<C0/(C0+C1-C5) NAP<0.55; apply these ratios to PAHs of coal, petroleum, sediment also have a good dispersion. Therefore, these ratios can be used for identify PAHs from coal gangue. Through the toxicity evaluation of coal gangue, the average Benzoapyrene toxicity equivalent concentration reached 194.60ng/g, in which a-PAH contributed most of the toxicity equivalent concentration. This study provides basic experimental data for the source of PAHs and reveals the possible ecological risks of PAHs in coal gangue.
Ball A, Truskewycz A. Polyaromatic hydrocarbon exposure:an ecological impact ambiguity[J]. Environmental Science & Pollution Research, 2013,20(7):4311-4326.
[2]
Shen M, Xing J, Ji Q, et al. Declining Pulmonary Function in Populations with Long-term Exposure to Polycyclic Aromatic Hydrocarbons-Enriched PM2.5[J]. Environ. Science Technology, 2018,52(11):6610-6616.
[3]
Xiao R, Bai J, Wang J, et al. Polycyclic aromatic hydrocarbons (PAHs) in wetland soils under different land uses in a coastal estuary:Toxic levels, sources and relationships with soil organic matter and water-stable aggregates[J]. Chemosphere, 2014,110:8-16.
[4]
刘志华,刘大锰,姚艳斌.燃煤产物中多环芳烃赋存规律及环境意义[J]. 煤炭科学技术, 2009,5:115-118. Liu Z H, Liu D M, Yao Y B. Distributed law and environment significance of polycyclic aromatic hydrocarbons in coal burning productao[J]. Coal Science and Technology, 2009,5:115-118.
[5]
马伦,陆大荣,梁汉东,等.神华长焰煤大分子结构特征的研究[J]. 燃料化学学报, 2013,41(5):513-522. Ma L, Lu D R, Liang H D, et al. Preliminary study on macromolecular structure characteristics of Shenhua long flame coal[J]. Journal of Fuel Chemistry and Technology, 2013,41(5):513-522.
[6]
吴国强,汪涛,王家伟,等.煤和煤矸石及其燃烧产物中稀土元素赋存形态研究[J]. 燃料化学学报, 2020,48(12):1498-1505. Wu G Q, Wang T, Wang J W, et al. Occurrence forms of rare earth elements in coal and coal gangue and their combustion products[J]. Journal of Fuel Chemistry and Technology, 2020,48(12):1498-1505.
[7]
Liu, H B, Liu Z L. Recycling utilization patterns of coal mining waste in China[J]. Resour Conserv Recycl, 2010,54(12):1331-1340.
[8]
BP. BP statistical review of world energy[Z]. 2019.
[9]
Sun Y, Fan J, Qin P, et al. Pollution extents of organic substances from a coal gangue dump of Jiulong Coal Mine, China[J]. Environmental Geochemistry and Health, 2009,31(1):81-89.
[10]
Yang Y R, Gao H F, Yue X F, et al. Polycyclic aromatic hydrocarbon (PAH) -containing soils from coal gangue stacking areas contribute to epithelial to mesenchymal transition (EMT) modulation on cancer cell metastasis[J]. Science of the Total Environment, 2017,580:632-640.
[11]
尚誉,杨丰隆,董轶茹,等.矸石山及其周边村庄土壤浸出液对大麦的毒性作用[J]. 环境科学, 2020,41(6):2936-2941. Shang Y, Yang F L, Dong Y R, et al. Toxicity of soil leachate from coal gangue and its surrounding village of barley (Hordeum vulgare)[J]. Environmental Science, 2020,41(6):2936-2941.
[12]
郭盛华.煤矸石污染与综合利用的途径[J]. 环境科学, 1985,16(6):27-31. Guo S H. Coal stone removal pollution and comprehensive utilization approach[J]. Environmental Science, 1985,16(6):27-31.
[13]
Benjamin Hindersmann, Christine Achten. Urban soils impacted by tailings from coal mining:PAH source identification by 59PAHs, BPCA and alkylated PAHs[J]. Environmental Pollution, 2018,242:1217-1225.
[14]
范维唐,杨锡禄.中国煤炭工业百科全书(地质·测量卷)[M]. 北京:煤炭工业出版社, 1996:456. Fan W T, Yang X L. China coal industry encyclop aedia(Geology & Survey volame)[M]. Beijing:China Coal Industry Publishing House, 1996:456.
[15]
樊景森,浑凌云,骈炜.峰峰五矿煤矸石山周围有机污染特征研究[J]. 环境工程, 2016,34(S1):828-832. Fan J S, Hun L Y, Pian W. Organic pollution of coal gangue dump in No.5caol mine in fengfeng,China[J]. Enviromental Engineering, 2016,34(S1):828-832.
[16]
冯精兰,翟梦晓,申君慧,等.超声萃取-高效液相色谱法测定沉积物中多环芳烃[J]. 理化检测(化学分册), 2012,48(3):308-311. Feng J L, Gai M X, Shen J H, et al. HPLC Determination of polycyclic aromatic hydrocarbons in sediment with ultrasonic extaction[J]. Physical Testing and Chemical Analysis(Part B:Chemical Analysis), 2012,48(3):308-311.
[17]
Carles P, Alejandra P, Josep R, et al. Analysis of alkyl and 2-6-ringed polycyclic aromatic hydrocarbons by isotope dilution gas chromatography/mass spectrometry:Quality assurance and determination in Spanish river sediments[J]. Journal of Chromatography A, 2006,1113(1/2):220-230.
Stout S A, Emsbo-Mattingly S D. Concentration and character of PAHs and other hydrocarbons in coals of varying rank-Implications for environmental studies of soils and sediments containing particulate coal[J]. Organic Geochemistry, 2008,39:801-819.
[20]
GB5751-86中国煤炭分类[S]. GB5751-86 Coal classification in China[S].
[21]
张小凤,文雪琴,杨亚丽.不同变质程度煤中夹矸中多环芳烃的分布特征[J]. 煤炭技术, 2016,35(11):180-182. Zhang X F, Wen X Q, Yang Y L. Distribution Characteristic of Polycyclic Aromatic Hydrocarbons(PAHs) in Different Coal Rank of Coals Gangue[J]. Coal Technology, 2016,35(11):180-182.
[22]
张黎明,周建伟,柴波,等.合山煤矸石堆周边土壤中多环芳烃的空间分布特征[J]. 生态与农村环境学报, 2014,30(5):652-657. Zhang L M, Zhou J W, Chai B, et al. Spatial Distribution of PAHs in Soils Around Coal Gangue Piles in Heshan[J]. Journal of Ecology and Rural Environment, 2014,30(5):652-657.
[23]
乔元栋,罗化峰,宁掌玄,等.煤矸石充填土壤中多环芳烃的迁移规律研究[J]. 中国煤炭, 2020,46(7):73-78. Qiao Y D, Luo H F, Ning Z X, et zl. Stugy on the migration rule of polycyclic aromatic hydrocarbons in the soil filled with coal gangue[J]. China Coal, 2020,46(7):73-78.
[24]
Li Y J, Wu Y D, Xu J, et al. Chemical characterization of particulate organic matter from commercial restaurants:Alkyl PAHs as new tracers for cooking.[J]. The Science of the Total Environment, 2017, 580:632-640.
[25]
陈刚,周潇雨,吴建会,等.成都市冬季PM2.5中多环芳烃的源解析与毒性源解析[J]. 中国环境科学, 2015,35(10):3150-3156. Chen G, Zhou X Y, Wu J H, et al. Source apportionment and toxicity quantitation of PM2.5-associated polycyclic aromatic hydrocarbons obtained from Chengdu, China.[J]. China Environmental Science, 2015,35(10):3150-3156.
[26]
Zhang Y, Chen Y, Li R, et al. Determination of PM2.5-bound polyaromatic hydrocarbons and their hydroxylated derivatives by atmospheric pressure gas chromatography-tandem mass spectrometry[J]. Talanta, 2019,195:757-63.
[27]
Nádudvari A, Fabiańska M J, Marynowski L, et al. Distribution of coal and coal combustion related organic pollutants in the environment of the Upper Silesian Industrial Region[J]. The Science of the Total Environment, 2018,628-629:1462-1488.
[28]
孙溶,陈颖军,韩勇,等.典型烟煤中游离态母体及烷基多环芳烃的含量和组成特征[J]. 地球化学, 2017,46(4):358-366. Sun R, Chen Y J, Han Y, et al. The concentration and composition characteristics of soluble parent and alkylated polycyclic aromatic hydrocarbons in typical bituminous coals[J]. Geochimica, 2017, 46(4):358-366.
[29]
Sigve S, Nina G, Rainer G L, et al. Source identification of paromatic hydrocarbons in sediments using GC/MS[J]. Environmental Science & Technology, 1983,17:282-286.
[30]
Mark B Y; Robie W M; Roxanne V, 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.
[31]
刘文静,李广坡,倪进治,等.土壤有机质组分中多环芳烃分配特征和生态风险[J]. 中国环境科学, 2020,40(4):1620-1627. Liu W J, Li G P, Ni J Z, et al. Distribution patterns and ecological risks of polycyclic aromatic hydrocarbons in different soil organic matter fractions[J]. China Environmental Science, 2020,40(4):1620-1627.
[32]
梅卫平,阮慧慧,吴昊,等.滴水湖水系沉积物中多环芳烃的分布及风险评价[J]. 中国环境科学, 2013,33(11):2069-2074. Mei W P, Ruan H H, Wu H, et al. Distribution and ecological risk assessment of polycyclic aromatic hydrocarbons in sediments from Dishui Lake water system[J]. China Environmental Science, 2013,33(11):2069-2074.
[33]
鲁垠涛,王雪雯,张士超,等.黄河全流域岸边表层土壤中PAHs的分布、来源及风险评估[J]. 中国环境科学, 2019,39(5):2078-2085. Lu Y T, Wang X F, Zhang S C, et al. Distribution, source and risk assessment of PAHs in surface soil of the Yellow River Basin[J]. China Environmental Science, 2019,39(5):2078-2085.
[34]
Ramachandran S D, Hodson P V, Khan C W, et al. Oil dispersant increases PAH uptake by fish exposed to crudeoil[J]. Ecotoxicology and Environmental Safety, 2004,59(3):300-308.
[35]
张娟,吴建芝,刘燕.北京市绿地土壤多环芳烃分布及健康风险评价[J]. 中国环境科学, 2017,37(3):1146-1153. Zhang J, Wu J Z, Liu Y. Polycyclic aromatic hydrocarbons in urban green space of Beijing:distribution and potential risk[J]. China Environmental Science, 2017,37(3):1146-1153.
[36]
Atmospheric quality standards and criteria[R]. Gouvernement du Québec, Canada, 2021.
[37]
Khalili N R, Scheff P A, Holse T. PAH source fingerprints for coke ovens, diesel and gasoline-engines,highway tunnels and wood combustion emissions[J]. Atmos. Environ., 1995,29(4):533-542.
[38]
Wirgin I, Waldman J R. Resistance to contaminants in North American fish populations.[J]. Mutat. Res., 2004,552(1/2):73-100.
[39]
Golzadeh N, Barst B D, Baker J M, et al. Alkylated polycyclic aromatic hydrocarbons are the largest contributor to polycyclic aromatic compound concentrations in traditional foods of the Bigstoneree Nation in Alberta, Canada[J/OL]. Environmental Pollution, https://doi.org/10.1016/j.envpol.2021.116625.
[40]
Risk assessment guidance for superfund (RAGS), Vol.I:Human health evaluation manual (part E), Supplemental guidance from dermal risk assessment[Z]. US EPA, 2004.