【摘要】 近年来,全氟烷基酸（perfluoroalkyl acids,PFAAs）在我国的各种环境介质中被广泛检出,对生态环境和人体健康构成了潜在威胁.本研究利用大流量主动采样器收集广州、太古、昆明、厦门、南昌、绵阳、南京、青岛、北京和天津等10个城市及五指山地区的大气颗粒物,利用被动采样技术收集除南京和天津外9个城市和地区的大气颗粒物,调查颗粒物中的全氟辛烷羧酸（perfluorooctanoic acid,PFOA）和全氟辛烷磺酸（perfluorooctane sulfonate acid,PFOS）的污染特征和来源.主动采样方法揭示了PFAAs的时空分布特征.空间分布上,10个典型城市中,PFOA浓度范围为0.08—25 pg·m^-3,0.11—36 ng·g^-1;PFOS浓度范围为(0.12—14 pg·m^-3,0.19—9.4 ng·g^-1),五指山PFOA(0.23—1.2 pg·m^-3,0.16—0.83 ng·g^-1)和PFOS(0.31—0.93 pg·m^-3,0.31—1.1 ng·g^-1)的浓度低于10个典型城市.PFOA和PFOS浓度整体上呈现东部>中部>西部>背景点的趋势.时间变化上,广州市大气颗粒物中PFOA浓度没有呈现显著的随时间的变化趋势,PFOS浓度在秋冬季(4.2±4.7 pg·m^-3,2.1±1.9 ng·g^-1)低于春夏季(6.3±3.9 pg·m^-3,4.7±1.6 ng·g^-1).五指山PFOS浓度在旱季(0.48±0.23 pg·m^-3,0.57±0.22 ng·g^-1)和雨季(0.52±0.24 pg·m^-3,0.56±0.27 ng·g^-1)处于同一水平.其他9城市PFAAs的浓度随时间变化趋势具有显著差异.10个典型城市PFAAs的来源主要与排放源的分布有关,背景点五指山主要受长距离迁移的影响.大气被动采样获得的PFAAs浓度与主动采样具有显著差异,较长的采样时间可能造成PFAAs的积累.在一定的时间和空间范围内,被动与主动采样获得的浓度变化趋势呈现一致规律,揭示了被动采样方法的适用性.PFOA的采样速率为18±16 m³·d^-1,PFOS的采样速率为3.1±2.4 m³·d^-1.针对PFAAs的被动采样捕集理论和适用范围还有待进一步研究.更多还原

【Abstract】 In recentyears,perfluoroalkyl acids（ PFAAs） have been detected in various-environmentalmedia,which pose potential threats to ecosystem and human health. In this study,high-volume active air samplers were deployed in 10 cities including Guangzhou,Taigu,Kunming,Xiamen,Nanchang,Mianyang,Nanjing,Qingdao,Beijing,Tianjin and 1 background site,Wuzhishan to collect particles in air. Passive air samplers were deployed in 9 sitesexcluding Nanjing and Tianjin.The concentrations,distribution and sources ofperfluorooctanoic acid（ PFOA） and perfluorooctane sulfonate acid（ PFOS） in the atmospheric particles were investigated in 11 sampling sites. The spatial distribution and time variations were revealed by the data obtained from active air sampling. In the 10 cities,the concentrations of PFOA varied from 0. 08 to 25 pg·m^-3,0. 11 to 36 ng·g^-1 and the concentrations of PFOS varied from 0.12 to 14 pg·m^-3,0.19 to 9.4 ng·g^-1. The concentrations of PFOA( 0. 23—1. 2 pg·m^-3,0. 16—0. 83 ng·g^-1) and PFOS( 0. 31—0. 93 pg·m^-3,0. 31—1.1 ng·g^-1) at Wuzhishan were lower than the 10 cities. PFOA and PFOS concentrations declined in the following order: the eastern >the middle >the western >the background sites. In Guangzhou,the concentrations of PFOA did not present significant time variations,and PFOS in autumn and winter( 4.2±4.7 pg·m^-3,2.1±1.9 ng·g^-1) was lower than that in spring and summer( 6.3±3.9 pg·m^-3,4.7±1.6 ng·g^-1). In Wuzhishan,the concentrations of PFOS in dry season( 0.48±0.23 pg·m^-3,0.57±0.22 ng·g^-1) and wet season( 0.52±0.24 pg·m^-3,0.56±0.27 ng·g^-1) wereat the same level.The time variations of PFAAs concentrations were significantly different in other 9 cities. The sources of PFAAs in atmospheric particles in cities were mainly related to the industrial and domestic emission,and the source in Wuzhishan was mainly related to the long range atmospheric transport.The concentrations of PFAAs obtained from passive air sampling were significantly different from those of active sampling,and the long sampling time might lead to the accumulation on the filter. In some specificsampling periods,thespatial distribution of PFAAs investigated by active and passive air sampling were consistent in some cities,which indicated the applicability of passive air sampling.The sampling speed of PFOA was 18±16 m³·d^-1,and the speed of PFOS was 3.1±2.4 m³·d^-1. More researches should be conducted about the theory of PFAAs trapping in particles and the applicability of passive air sampling.更多还原