YIC-IR  > 中科院烟台海岸带研究所知识产出
全(多)氟化合物在典型氟工业园区河流中的污染特征研究
Alternative TitleDistribution characteristics of perfluoroalkyl and polyfluoroalkyl substances (PFASs) in rivers around fluorine industrial parks
孙琳婷
Subtype硕士
Thesis Advisor唐建辉
2020-11-25
Degree Grantor中国科学院大学
Place of Conferral北京
Degree Name工程硕士
Degree Discipline环境工程
Keyword小清河 全(多)氟化合物 污染水平 分配系数 工业园
Abstract全(多)氟化合物(Perfluoroalkyl and Polyfluoroalkyl substances, PFASs)凭借其独特的理化性质在生产与生活中应用广泛,同时也导致其在环境中普遍存在。目前,PFASs在全球大气、水体、沉积物、生物体等各种环境介质中被广泛检出,并且部分单体能够通过食物链富集放大,对生态系统和人类健康造成极大威胁,引起国际关注。随着PFOS和PFOA相继被列入《斯德哥尔摩公约》,短链PFASs及新型PFASs的生产和使用逐步扩大,且在环境中不断检出,成为新的研究热点。 本研究采取固相萃取(SPE)富集结合超高效液相色谱/质谱联用(UPLC-MS/MS)检测的手段,对河流-近海环境中21种PFASs的污染特征进行分析。本研究的工作分为两部分开展:1. 以不同氟工业园区周边河流为研究对象,对比分析辽宁细河、山东小清河、长江江苏段表层沉积物中PFASs污染特征。2. 以三个区域中污染最严重的小清河为研究对象,分析整个流域PFASs污染特征及悬浮颗粒物(SPM)-水之间分配规律。具体结论如下: 1. 三个氟工业园附近河流表层沉积物中,PFASs污染水平和组成特征均有显著差异。小清河表层沉积物PFASs是三个区域中含量最高的,其次为细河,最后为长江。小清河表层沉积物中全氟辛酸(PFOA)和六氟环氧丙烷二聚酸(HFPO-DA)为优势污染物;细河表层沉积物中主要污染物是全氟丁烷磺酸(PFBS)和HFPO-DA;长江表层沉积物中全氟十四酸(PFTeDA)和6:2氟调磺酸(6:2 FTS)为主要污染物。不同区域河流河流沉积物中PFASs的浓度水平与组成特征的差异与不同工业园区规模、生产工艺、产能和生产模式有关。三个区域表层沉积物中PFASs含量与沉积物理化性质相关性不明显,说明PFASs在沉积物中的转移和富集过程受多种因素共同作用。 2. 小清河表层水体和SPM中均存在PFASs污染。小清河表层水体PFASs浓度范围为94.0 ~ 444000 ng/L,主要污染物为PFOA、PFHpA和HFPO-TA。SPM中,PFASs浓度范围为34.6 ~ 94900 ng/g dw,HFPO-TA和PFOA是主要的污染物。PFASs污染水平在氟化物工业园下游的东竹龙支流X10站位急剧上升,说明点源排放是造成PFASs污染的主要原因,且对小清河干流PFASs污染造成影响。PFASs在SPM水两相的分配与碳链长度及污染物性质有关。研究结果发现,长链PFCAs和PFSAs更容易分配在SPM中。此外,水体中SPM的浓度升高会对PFASs的分配行为产生影响。 通过对比不同工业园区周边河流表层沉积物中PFASs的污染水平及组成的不同,发现不同工业园的规模、产能和生产模式都有可能对其周边环境介质产生不同的影响,化合物性质、沉积物理化性质在不同区域对PFASs影响也存在差异。其中沉积物中PFASs污染最为严重的小清河,其水体中PFASs污染直接受点源排放的影响,且PFASs在SPM-水两相之间的分配行为受化合物性质、水体中SPM浓度影响。因此,在后续研究PFASs在水环境中的分布、分配以及迁移转化要综合考虑点源特点、化合物性质、环境介质理化性质等因素,以期对环境中PFASs做出更加全面详细的分析。
Other AbstractPFASs are widely used in industrial and domestic products owing to their unique physical and chemical properties. At present, PFASs are ubiquitously presented in the atmosphere, water, sediments, organisms and other environmental media all over the world. They can be bioaccumulated and biomagnified through the food chain, posing a great threat to the ecosystem and human health, and hence attracting international attention. As PFOS and PFOA have been included in the Stockholm Convention, the production and use of short-chain PFASs and novel PFASs have gradually increased, and resulted they been frequently detected in the environment, becoming a new research hotspot. In this study, solid phase extraction (SPE) enrichment combined with ultra-high performance liquid chromatography/mass spectrometry (UPLC-MS/MS) detection methods were used to analyze the distribution characteristics of 21 PFASs in the river-estuary environment. This research includes two parts: 1. To screen the PFAS contamination status and distribution characteristics by analysis riverine surface sediments surrounding three different fluorine industrial parks, i.e., Xihe River in Liaoning province, Xiaoqing River in Shandong province, and Yangtze River in Jiangsu Province; 2. Taking the most polluted Xiaoqing River among the three regions as a case study, to analyze the distribution characteristics of PFASs and the partition coefficients of PFASs between soluble phase/suspended particulate matter (SPM) in the entire river basin. The specific conclusions are as follows: 1. The concentration and composition of PFASs varied largely in the surface sediments among the three rivers near the fluorine industrial parks. Xiaoqing River showed the highest PFASs levels, followed by the Xihe River, and finally the Yangtze River. The dominant compounds were PFOA and HFPO-DA in the Xiaoqing River, PFBS and HFPO-DA in the Xihe Rvier, and PFTeDA and 6:2 FTS in the Yangtze River, respectively. This is mainly attributed to the capacities, technical processes, and production mode in different industrial parks. The correlation between PFASs and physical and chemical properties of the sediments were complicated among the three regions, indicating that the transfer and enrichment processes of PFASs in the sediments were affected by many factors. 2. Extremely high levels of PFASs were detected in the surface water and SPM of Xiaoqing River. The concentration of PFASs in the surface waters of Xiaoqing River ranges from 94.0 to 444,000 ng/L, and the dominant pollutants are PFOA, PFHpA and HFPO-TA. In SPM, the concentration of PFASs ranges from 34.6 to 94,900 ng/g dw, and HFPO-TA and PFOA are the main pollutants. The concentration of PFASs rose sharply at station X10 on the Dongzhulong tributary, which locates downstream of the fluoride industrial park, indicating that point source emissions are the main cause of PFASs pollution and have an impact on the PFASs pollution of the main stream of the Xiaoqing River. The partition coefficients of PFASs between the SPM and soluble phase were related to the lengths of the carbon chain and the physicochemical properties of the pollutants. Long-chain PFCAs and PFSAs were prone to adsorb to SPM. In addition, the increase in the concentration of SPM in water will affect the distribution behavior of PFASs. By comparing the concentration and composition of PFASs in the surface sediments of the rivers surrounding different industrial parks, it is found that the factory capacities, chemical processes and production mode of different industrial parks may have different effects on the surrounding environmental media. In different regions, the impact on PFASs of the nature of the compound and the physical and chemical is also different. Among the three regions, Xiaoqing River showed the most serious PFASs contamination, and the concentration of PFASs in the water is directly affected by point source emissions. The distribution of PFASs between the SPM-water phases is affected by the nature of the compound and the concentration of SPM in the water. Therefore, in the follow-up study of the distribution, allocation, migration and transformation of PFASs in the water environment, it is necessary to comprehensively consider factors such as point source characteristics, compound properties, and physical and chemical properties of environmental media, in order to make a more comprehensive and detailed analysis of PFASs in the environment.
Subject Area环境科学技术
MOST Discipline Catalogue工学::环境科学与工程(可授工学、理学、农学学位)
Pages120
Language中文
Document Type学位论文
Identifierhttp://ir.yic.ac.cn/handle/133337/25309
Collection中科院烟台海岸带研究所知识产出
Recommended Citation
GB/T 7714
孙琳婷. 全(多)氟化合物在典型氟工业园区河流中的污染特征研究[D]. 北京. 中国科学院大学,2020.
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