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黄河三角洲悬浮颗粒物中抗生素的赋存特征及生态风险评价

[Occurrence Characteristics and Ecological Risk Assessment of Antibiotics in Suspended Particulate Matter in the Yellow River Delta].

作者信息

Yuan Zhen, Zhang Shu-Xiang, Li Xin-Bin, Che Chun-Guang, Wang Qi-Yuan, Xia Zheng-Qi, Wang Kun, Sun Ying-Jie

机构信息

School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266520, China.

Yellow River Estuary Management Station, Yellow River Delta National Nature Reserve, Dongying 257231, China.

出版信息

Huan Jing Ke Xue. 2025 Jul 8;46(7):4273-4284. doi: 10.13227/j.hjkx.202406028.

DOI:10.13227/j.hjkx.202406028
PMID:40677047
Abstract

To investigate the distribution and ecological risks of antibiotics in the aquatic environment of the Yellow River Delta (YRD), the pollution characteristics of 45 typical antibiotics, including fluoroquinolones, sulfonamides, tetracyclines, and macrolides were determined in water and suspended particulate matter (SPM) samples collected from the lower reaches of the YRD, YRD Nature Reserves, and the YRD Estuary. This study use a high performance liquid chromatography tandem triple quadrupole mass spectrometry to measure the concentrations. The results showed that 12 and 18 antibiotics were detected at concentration levels in the range of N.D.-4 249.79 ng·L and N.D.-8 535.39 ng·g in the water and SPM samples, respectively. Among them, norfloxacin, enoxacin, doxycycline, pefloxacin, and sarafloxacin, belonging to fluoroquinolones and tetracyclines, were mostly detected; for the sulfonamides, the detection rate and concentration levels were relatively low, and macrolides were not detected in any samples. Moreover, due to the significant influences of human activities, the levels of antibiotic pollution were generally higher downstream than those upstream in the YRD water bodies. The levels of antibiotic pollution were positively correlated with the salinity of the waters in the nearby estuary. Conversely, the total concentrations of target antibiotics in the suspended particulate matter (SPM) were higher upstream than those downstream, which were consistent with the content of SPM along the sampling sites. Furthermore, the partition coefficient () of the detected antibiotics between water and SPM were calculated, showing that the (L·kg)values were in the range of 1.2×10 (doxycycline)-8.7×10 (sarafloxacin). These results suggested that the detected antibiotics tended to be associated with SPM once entering the investigated area. Of particular note, it was observed that the values followed the rank order: fluoroquinolones>tetracycline>sulfonamides, and there was a significant spatial variability. The correlation analysis of and water environment factors showed that the partition of target antibiotics in the water-SPM interface was largely dependent on the properties of organic matter. In addition, the microstructure and composition of SPM also played an important role in the interaction between the antibiotics and SPM. The ecological risk assessment results showed that norfloxacin in water presented a high risk to aquatic organisms, doxycycline presented a moderate risk to algae and invertebrates, chlortetracycline and sulfadimethoxine had a low risk to invertebrates with a low trophic level, and other antibiotics had a small risk. However, when considering the multiple risk of simultaneous pollutants, all sites appeared as high risk and require further attention.

摘要

为调查黄河三角洲(YRD)水环境中抗生素的分布及生态风险,在黄河三角洲下游、黄河三角洲自然保护区和黄河三角洲河口采集的水和悬浮颗粒物(SPM)样本中,测定了45种典型抗生素(包括氟喹诺酮类、磺胺类、四环素类和大环内酯类)的污染特征。本研究采用高效液相色谱串联三重四极杆质谱法测定浓度。结果表明,在水和SPM样本中分别检测到12种和18种抗生素,浓度范围分别为未检出(N.D.)-4 249.79 ng·L和未检出(N.D.)-8 535.39 ng·g。其中,属于氟喹诺酮类和四环素类的诺氟沙星、依诺沙星、多西环素、培氟沙星和沙拉沙星检出频率最高;磺胺类的检出率和浓度水平相对较低,且在任何样本中均未检出大环内酯类。此外,由于人类活动的显著影响,黄河三角洲水体中抗生素污染水平总体上是下游高于上游。抗生素污染水平与附近河口水体盐度呈正相关。相反,悬浮颗粒物(SPM)中目标抗生素的总浓度上游高于下游,这与沿采样点的SPM含量一致。此外,还计算了所检测抗生素在水和SPM之间的分配系数(),结果表明(L·kg)值在1.2×10(多西环素)-8.7×10(沙拉沙星)范围内。这些结果表明,所检测的抗生素一旦进入研究区域,往往会与SPM结合。特别值得注意的是,观察到值的排序为:氟喹诺酮类>四环素类>磺胺类,且存在显著的空间变异性。与水环境因子的相关性分析表明,目标抗生素在水- SPM界面的分配很大程度上取决于有机物的性质。此外,SPM的微观结构和组成在抗生素与SPM的相互作用中也起着重要作用。生态风险评估结果表明,水中的诺氟沙星对水生生物具有高风险,多西环素对藻类和无脊椎动物具有中度风险,金霉素和磺胺二甲氧嘧啶对低营养级无脊椎动物具有低风险,其他抗生素风险较小。然而,考虑到同时存在污染物的多重风险时,所有站点均呈现高风险,需要进一步关注。

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