蓟运河流域PPCPs时空异质性与健康风险评估

Spatiotemporal heterogeneity and health risk assessment of PPCPs in the Jiyun River Basin

  • 摘要: 为阐明天津市蓟运河流域表层水体中典型药品和个人护理品(PPCPs)的污染赋存特征与环境风险,本研究选取10类57种PPCPs为目标物,于2024年枯、丰水期在流域12个点位采集表层水样,采用固相萃取-超高效液相色谱-串联质谱技术分析其污染水平与时空分布规律,参照世界卫生组织与欧盟风险评估技术指导文件规范,采用风险商值法开展人体健康与水生生态风险评价。结果表明:57种目标物中共有17种被不同程度检出,检出浓度范围为N.D.(未检出)~720.57 ng/L,其中磺胺甲噁唑、咖啡因(CAF)、1,7-二甲基黄嘌呤(DTX)检出率均为100%;水体ΣPPCPs总浓度丰水期高于枯水期,空间上丰水期污染呈现中游>下游>上游的趋势,枯水期呈现下游>中游>上游的趋势;相关性分析显示DTX与ΣPPCPs呈极显著正相关(r=0.787, p<0.01),表明生活污水输入是流域PPCPs污染的重要来源。风险评价显示,目标PPCPs经饮水暴露对各年龄段人群均无显著健康风险(累计健康风险商2.24×10-4~1.68×10-2),0~3个月婴儿为最敏感人群;水生生态风险存在显著时空分异,枯水期风险高于丰水期,罗红霉素与CAF为流域优先管控污染物。

     

    Abstract: To elucidate the contamination occurrence characteristics and environmental risks of typical pharmaceuticals and personal care products (PPCPs) in the surface water of the Jiyun River Basin in Tianjin, we selected 57 PPCPs from 10 categories as target compounds. Surface water samples were collected from 12 sampling sites in the basin during the dry and wet seasons of 2024. Solid-phase extraction coupled with ultra-performance liquid chromatography-tandem mass spectrometry (SPE-UPLC-MS/MS) was employed to analyze their pollution levels and spatiotemporal distribution patterns. In accordance with the World Health Organization (WHO) guidelines and the European Commission Technical Guidance Document on Risk Assessment, the risk quotient method was used to assess the human health and aquatic ecological risks of target compounds. The results showed that 17 of the 57 target PPCPs were detected at various levels, with concentrations ranging from not detected (N.D.) to 720.57 ng/L. Among them, sulfamethoxazole, caffeine (CAF), and 1,7-dimethylxanthine (DTX) exhibited a 100% detection frequency. The total concentration of ΣPPCPs was higher in the wet season than in the dry season. Spatially, the pollution level followed the order of midstream > downstream > upstream in the wet season, and downstream > midstream > upstream in the dry season. Correlation analysis showed that DTX had an extremely significant positive correlation with ΣPPCPs (r=0.787, p<0.01), indicating that domestic sewage input was an important source of PPCPs pollution in the basin. The risk assessment indicated that the target PPCPs posed no significant health risk to people of all age groups via drinking water exposure, with the cumulative health risk quotient ranging from 2.24×10-4 to 1.68×10-2, and infants aged 0~3 months were the most sensitive group. Aquatic ecological risk exhibited significant spatiotemporal heterogeneity, with higher risk in the dry season than in the wet season. Roxithromycin and CAF were the priority control pollutants in the basin.

     

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