河流不同分子量溶解性有机质对全氟化合物赋存形态的影响

张杰; 赵璞君; 夏星辉

doi:10.13198/j.issn.1001-6929.2022.06.07

河流不同分子量溶解性有机质对全氟化合物赋存形态的影响

doi: 10.13198/j.issn.1001-6929.2022.06.07

北京师范大学环境学院，水沙科学教育部重点实验室，水环境模拟国家重点实验室，北京　100875

基金项目: 国家自然科学基金重点项目(No.52039001, 92047303)

详细信息

作者简介:
张杰（1992-），男，山东泰安人，zhang_jie@mail.bnu.edu.cn

通讯作者:
夏星辉(1971-)，女，湖南汨罗人，教授，博士，博导，主要从事流域水环境研究，xiaxh@bnu.edu.cn

中图分类号: X522
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出版历程
- 收稿日期: 2022-03-15
- 修回日期: 2022-05-19

Effects of Different Molecular Weight Dissolved Organic Matter on Occurrence Form of Polyfluoroalkyl Substances in River

Key Laboratory of Water and Sediment Sciences of Ministry of Education, State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, China

Funds: Key Program of the National Natural Science Foundation of China (No.52039001, 92047303)

摘要

摘要: 目前有关水体全氟化合物(PFASs)赋存特征的研究主要集中于总溶解态，对溶解性有机质(DOM)结合态PFASs的研究较为匮乏，尤其忽视了不同分子量DOM对PFASs赋存形态的影响. 为阐明河流上覆水体不同分子量DOM对PFASs赋存形态的影响，本文以长江干支流为例，分析了河流上覆水体11种典型PFASs (C4~C12)的浓度及组成，研究了不同分子量DOM结合态PFASs的赋存特征. 结果表明：①长江上覆水体中PFASs的平均浓度为52.6 ng/L，其中全氟戊酸(PFPeA)和全氟己酸(PFHxA)是最主要的单体污染物；由于受点源污染的影响，武汉段PFASs总溶解浓度及其单体浓度均显著高于其他采样点. ②长江上覆水体中DOM的浓度范围为0.08~3.84 mg/L (以C计)，将水体DOM按分子量分离为<1 kDa、1~3 kDa、3~5 kDa、5~10 kDa和>10 kDa五种组分，各采样点中<1 kDa的溶解性有机碳(DOC)浓度(1.56~3.84 mg/L)显著高于其他分子量的DOC浓度. ③对于所检出的PFASs，<1 kDa DOM结合态PFASs (含自由溶解态)的浓度亦显著高于其他分子量DOM结合态PFASs的浓度，且其占水体总溶解态PFASs的比例均在85%以上，说明水体DOM结合态PFASs具有较高的生物有效性. 研究显示，水体不同分子量DOM结合态PFASs的赋存特征存在差异，因此对水体PFASs进行生态风险评价时需综合考虑不同分子量DOM结合态的含量及其生物有效性.
- 长江 /
- 全氟化合物(PFASs) /
- 溶解性有机质(DOM) /
- 分子量 /
- 赋存形态
Abstract: At present, studies on the distribution of polyfluoroalkyl substances (PFASs) in the aquatic environment mainly focus on their total dissolved concentration, while the studies about PFASs associated with dissolved organic matter (DOM) is scarce, especially there is a lack of research on the effects of DOM with different molecular weights on the occurrence form of PFASs. To clarify the effects of DOM with different molecular weights on the occurrence form of PFASs in overlying water of rivers, the concentrations and composition of eleven PFASs (C4-C12) in overlying water of the Yangtze River were analyzed and the occurrence characteristics of PFASs associated with different molecular weight DOM were explored. The results showed that: (1) The average total dissolved concentration of PFASs in the overlying water of the Yangtze River was 52.6 ng/L, and perfluoropentanoic acid (PFPeA) and perfluorohexanoic acid (PFHxA) were the main monomer pollutants. Due to the influence of point source pollution, the total dissolved concentration and monomer concentration of PFASs in Wuhan were significantly higher than those in other sampling sites. (2) The concentration of DOM in the overlying water of the Yangtze River ranged from 0.08 mg/L to 3.84 mg/L. DOM was separated into <1 kDa, 1-3 kDa, 3-5 kDa, 5-10 kDa and >10 kDa by molecular weight. The concentration (1.56-3.84 mg/L) of dissolved organic carbon (DOC) of <1 kDa was significantly higher than that of other molecular weights. (3) For the detected PFASs, the concentration of PFASs associated with <1 kDa DOM (including freely dissolved PFASs) was significantly higher than that associated with other molecular weights DOM, accounting for more than 85% of the total dissolved PFASs in overlying water, indicating that the PFASs associated with DOM in overlying water had high bioavailability. This study shows that there are differences in the occurrence characteristics of PFASs associated with different molecular weight DOM in overlying water. Therefore, the concentration and bioavailability of PFASs associated with different molecular weight DOM should be considered comprehensively when conducting ecological risk assessment for PFASs in overlying water.
- the Yangtze River /
- polyfluoroalkyl substances (PFASs) /
- dissolved organic matter (DOM) /
- molecular weight /
- occurrence form

HTML全文

图 1 不同采样点上覆水体PFASs总溶解态的浓度

注：YB为宜宾段；LZ为泸州段；CQ为重庆段；HC为合川段(嘉陵江)；YC为宜昌段；CS为长沙段(湘江)；ZX为钟祥段(汉江)；WH为武汉段；NC为南昌段(赣江)；DT为大通段.

Figure 1. Concentrations of total dissolved PFASs in overlying water at different sampling sites

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图 2 不同采样点上覆水体中不同分子量的DOC浓度

Figure 2. Concentration of DOC with different molecular weights in overlying water at different sampling sites

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图 3 不同采样点上覆水体中不同分子量DOM结合态PFASs的浓度

Figure 3. Concentrations of PFASs associated with different molecular weight DOM in the overlying water at different sampling sites

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图 4 水体总溶解态中不同分子量DOM结合态PFASs的吸附贡献率

注：<1 kDa DOM结合态PFASs中含自由溶解态.

Figure 4. Adsorption contribution rate of PFASs associated with different molecular weight DOM in total dissolved water

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表 1 我国主要河流上覆水体PFASs总溶解态的浓度比较

Table 1. Comparison of total dissolved PFASs in overlying water from different rivers in China

采样区域	PFASs总溶解态浓度/(ng/L)		数据来源
采样区域	范围	平均值	数据来源
辽河	1.4~131	43.6	文献[27]
黄河干流	44.7~263.0	—	文献[23]
黄河支流	79.9~1 526.0	—	文献[23]
大运河	7.4~153.5	40.5	文献[28]
拉萨河	0.1~1.7	0.3	文献[29]
岷江	1.5~30.2	11.2	文献[30]
黄浦江	39.8~596.2	226.3	文献[31]
长江重庆段	52.3~69.1	—	文献[25]
长江重庆段	1.5~61.9	23.9	文献[32]
长江宜昌段	4.8~6.1	—	文献[33]
长江江苏至上海段	31.0~902.0	—	文献[33]
长江九江段	46.2~157.6	88.5	文献[34]
长江南昌段	146.2~586.2	322.1	文献[34]
长江干支流	31.8~117.0	52.6	该研究

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