胶州湾入海河流和排污口全氟多氟化合物的污染状况及来源解析  

Pollution Status and Source Analysis of Per-and Polyfluoroalkyl Substances in Rivers and Sewage Outlets of Jiaozhou Bay

作　　者：王瑶瑶 李俊龙[3] 李凤超[4] 李宏观 张明政 王晓雪 罗忻 梁生康 Wang Yaoyao;Li Junlong;Li Fengchao;Li Hongguan;Zhang Mingzheng;Wang Xiaoxue;Luo Xi;Liang Shengkang(College of Chemistry and Chemical Engineering,Ocean University of China,Qingdao 266100,China;The Key Laboratory of Marine Chemistry Theory and Technology,Ministry of Education,Ocean University of China,Qingdao 266100,China;China National Environmental Monitoring Centre,Beijing 100012,China;Shandong Weifang Ecological Environmental Monitoring Centre,Weifang 261000,China;Technology Center of Qingdao Customs,Qingdao 266000,China)

机构地区：[1]中国海洋大学化学化工学院,山东青岛266100 [2]中国海洋大学海洋化学理论与工程技术教育部重点实验室,山东青岛266100 [3]中国环境监测总站,北京100012 [4]山东省潍坊生态环境监测中心,山东潍坊261000 [5]青岛海关技术中心,山东青岛266000

出　　处：《中国海洋大学学报(自然科学版)》2025年第3期55-69,共15页Periodical of Ocean University of China

基　　金：崂山实验室“十四五”重大项目(LSKJ202203901);中央高校基本科研业务费专项(202262009)资助。

摘　　要：全氟多氟化合物(PFASs)是一类具有强环境持久性和高生物富集性的新污染物。环湾地区人类活动密集,水环境中PFASs的分布和风险备受关注。本研究于2022年8月(丰水期)和2023年4月(枯水期)分别采集了环胶州湾7条河流入海口和4个直排海城镇生活污水处理厂排污口样品,采用高效液相色谱串联质谱法分别测定溶解态和颗粒态PFASs的组成和含量。结果显示,丰水期和枯水期入湾河流和排污口水体中分别检出18种和16种溶解态PFASs,主要组分为全氟羧酸;丰水期和枯水期分别检出23种和25种颗粒态PFASs,以全氟磺酸及新兴替代物为主,六氟环氧丙烷二聚体羧酸(HFPO-DA)、6∶2氟调磺酸(6∶2FTSA)等新兴全氟多氟替代物均被检测到,说明环湾河流和废水普遍受到PFASs污染。丰水期环湾河流和排污口中溶解态和颗粒态总PFASs(∑PFASs)浓度均值均低于枯水期,表明入海河流径流对PFASs具有稀释作用。PFASs颗粒态-溶解态分配系数为2.05~4.10,随碳链长度的增加而增大,PFASs碳链越长疏水性越强,越容易被吸附到颗粒物上。丰水期胶州湾总PFASs入海通量为7.40 kg/d,高于枯水期的1.89 kg/d,其中,大沽河入海通量占比最高,丰水期和枯水期分别达到81.2%和83.6%。基于PFASs比值特征和主成分分析表明,入湾河流和排污口PFASs主要来源于氟化物制造、消防泡沫、纸包装、印刷等行业。重点污染区块位于娄山河排污单元、镰湾河排污单元和大沽河排污单元。丰水期入湾河流和排污口PFASs均为无风险,枯水期镰湾河、娄山河PFOA为低生态风险,其余入海河口PFASs均无风险。Per-and polyfluoroalkyl(PFASs)substances are a new class of pollutants with environmental persistence and high bioconcentration.The distribution and risk of PFASs in the environment are of great concern in the Bay region,where human activities are intensive.In this study,samples were collected from seven rivers and four sewage outlets in Jiaozhou Bay(JZB)in August 2022(wet season)and April 2023(dry season),respectively.The composition and content of PFASs in the dissolved and particulates were determined by high-performance liquid chromatography-tandem mass spectrometry.The results showed that 18 and 16 PFASs were detected in the dissolved during the wet and dry seasons,respectively,with perfluorinated carboxylic acids(PFCAs)as the main components.There were 23 and 25 PFASs detected in the particulate during the wet and dry seasons,respectively,with perfluorinated sulfonic acids(PFSAs)and emerging alternatives as the main components.In addition,HFPO-DA and 6∶2 FTSA were detected in both media,suggesting that the rivers and wastewater around the bay were generally contaminated with PFASs.The mean concentrations of total dissolved and particulate PFASs(∑PFASs)in the rivers and outfalls around the bay were lower in the wet period than in the dry period,indicated that the runoff from the rivers into the sea had a dilution effect on PFAS.The particle state-dissolved state partition coefficients of PFASs ranged from 2.05 to 4.10,which increased with the increase of carbon chain length,and the longer the carbon chains of PFASs,the more hydrophobic they were,and the more likely they were to be adsorbed onto particulate matter.The∑PFASs flux into JZB reached 7.40 kg/d during the wet season,much higher than the 1.89 kg/d during the dry season.The Dagu River had the highest percentage of fluxes into the sea,reaching 81.2%and 83.6%in the wet and dry seasons,respectively.Based on the characteristics of the PFASs ratio and the results of principal component analysis,the PFASs mainly originated from point source discharge

关 键 词：胶州湾 河流和排污口 全氟多氟化合物 污染状况 通量 来源解析 

分 类 号：P734[天文地球—海洋化学]