上海市饮用水中全氟化合物的污染现状及风险评估

Assessment of contamination and health risk of perfluoroalkyl substances in drinking water in Shanghai

  • 摘要:
    背景 全氟化合物(PFAS)具有持久性、蓄积性、迁移性和毒性,广泛存在于各类水体中,存在饮水途径摄入的风险。
    目的 研究上海市饮用水中PFAS的污染状况,并对其进行风险评估。
    方法 选取长江口水源地和黄浦江上游水源地采集水源水,分别编号为A和B。以A为水源的水厂制水工艺有常规处理、深度处理2种,分别随机抽取1个水厂采集出厂水;以B为水源的水厂均已改为深度处理,因此随机抽取1个水厂采集出厂水。于2019年10月(平水期)、2019年12月(枯水期)、2020年7月(丰水期)分别进行采样,每个地点采集2个平行样品,采样量为1 L,容器为棕色聚丙烯塑料瓶。采用固相萃取-超高效液相色谱串联质谱法,测定水样中的23种全氟化合物,运用美国环境保护署(EPA)推荐的非致癌物质健康风险模型进行风险评估。
    结果 23种目标物中,水源水和出厂水中100%检出的分别为14种和11种,检出物均包括全氟羧酸类和全氟磺酸类两类物质;未检出的PFAS分别为9种和12种,均为全氟酰胺类化合物。两类水体中ΣPFAS(检出总浓度)为15.52~118.44 ng·L-1,其中全氟辛酸(PFOA)和全氟丁酸(PFBA)为主要污染物,最高浓度分别为34.79、29.99 ng·L-1,且PFOA和全氟辛烷磺酸(PFOS)的浓度均未超过EPA规定的饮用水阈值(70 ng·L-1)。B水源的ΣPFAS是A水源的2.7倍,除全氟壬烷磺酸(PFNS)在A水源稍高外,B水源的检出物浓度均高于A水源。A水源的PFAS含量在不同时期差异较小,B水源则表现为枯水期>平水期>丰水期。水处理工艺对A水源中的PFAS有较好的去除效果,其中常规处理去除率21.97%,深度处理为64.29%;对B水源的去除效果不明显,处理前后含量变化不大。PFOA、PFOS的个人年超额风险均低于国际辐射防护委员会推荐的最大可接受风险(10-6·年-1)。
    结论 上海市饮用水中存在一定程度的PFAS污染。PFOS和PFOA经饮水途径对人体健康造成的个人年超额风险较低,低于国际辐射防护委员会推荐的最大可接受水平。

     

    Abstract:
    Background Perfluoroalkyl substances (PFAS) with their persistence, accumulation, migration, and toxicity are widely found in various water bodies, indicating potential human exposure risk via drinking water.
    Objective This study aims to analyze the pollution status of PFAS in drinking water in Shanghai and assess relevant human health risk.
    Methods Source water samples were collected from two water sources (A and B) in Shanghai, including the Yangtze estuary water source and the Huangpu River upstream water source. According to water production process, treated water samples were collected from one routine treatment water plant and one deep treatment water plant which both used water source A, as well as from one deep treatment water plant which used water source B. Samples were collected in October 2019 (level period), December 2019 (dry period), and July 2020 (wet period) respectively, with 2 parallel samples from each site, and stored in 1-litre brown polypropylene plastic containers. A total of 23 PFAS were determined by solid phase extraction and ultra high performance liquid chromatography tandem-mass spectrometry. Then the risks of non-carcinogenic chemicals was evaluated by US Environmental Protection Agency (EPA) health risk assessment models.
    Results Among the 23 target substances, 14 and 11 kinds of PFAS were detected in all source water and treated water samples (100%), respectively, including perfluorinated carboxylic acid and perfluorinated sulfonic acid; 9 and 12 kinds of PFAS were not detected, respectively, and all were perfluoroamides. The total concentration of PFAS (ΣPFAS) in two types of water was 15.52 to 118.44 ng·L-1, the highest concentrations of dominant perfluorooctanoic acid (PFOA) and perfluorobutanoic acid (PFBA) were 34.79 and 29.99ng·L-1, respectively, and the concentrations of PFOA and perfluorooctane sulfonate (PFOS) did not exceed the drinking water threshold (70 ng·L-1) stipulated by US EPA. The ΣPFAS concentration of water source B was 2.7 times that of water source A. Except the perfluoro-1-nonanesulfonate (PFNS) slightly higher in water source A, the concentrations of detected substances in water source B were significantly higher than those in water source A. The concentration of PFAS in water source A showed little difference in different periods, while that in water source B was shown as dry period > level period > wet period. The PFAS in water source A were removed effectively by water treatment processes, as the removal rate was 21.97% by conventional treatment and 64.29% by deep treatment. The removal effect in water source B was not obvious, and the content of contaminants before and after treatment had little changes. The annual personal excess risks of PFOA and PFOS were lower than the maximum acceptable risk (10-6 per year) recommended by the International Committee of Radiological Protection (ICRP).
    Conclusion There is slight PFAS contamination in Shanghai's drinking water. The annual personal excess risks of PFOS and PFOA via drinking water are low and below the maximum acceptable level recommended by the ICRP.

     

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