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题名: 空气中多氯萘和多氯联苯的分布特征研究
作者: 朱青青1
学位类别: 博士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 郑明辉
关键词: 多氯萘,多氯联苯,空气,颗粒物,分布特征 ; PCNs, PCBs, Atmosphere, Particle, Distribution Characteristics.
其他题名: Distributions of Polychlorinated Naphthalenes and Polychlorinated Biphenyls in Air
学位专业: 环境科学
中文摘要: 多氯萘(PCNs)和多氯联苯(PCBs)是两类结构性质相似的持久性有机污 染物,具有高毒性、持久性和生物累积性,对人体健康和环境构成潜在威胁。空 气是其在环境中迁移转化的重要介质,也是人体暴露的主要途径之一。近年来, 关于空气中PCNs和PCBs的污染水平、环境行为及污染来源等研究已广泛开展, 但是由于采样方法的差异,监测数据间的可比对性研究还未明确。且目前关于 PCNs的研究大多集中于气相介质,缺乏对 PCNs气固相分配的全面了解,尤其 是 PCNs在不同粒径颗粒物上的分布特征研究尚属空白。同时,PCBs的粒径分 布特征研究也鲜有报道。因此,开展空气中 PCNs和 PCBs的浓度水平、气固相 分配及粒径分布特征的研究将有助于更好地了解其环境行为,从而进一步科学评 估人体呼吸暴露风险。 本论文首先开展了大气中 PCNs和 PCBs监测技术的可比对性研究,在此基 础上,以环境大气和再生铜冶炼车间空气为研究对象,系统开展了 PCNs和 PCBs 的污染水平、气固相分配及粒径分布特征研究。主要研究结果如下: 1、对比研究了大气中 PCNs和 PCBs的浓度水平及分布特征,表明不同的大 流量空气采样方法具有可比对性。利用不同的大流量空气采样器在北京城市生态 系统研究站采集空气样品,分别为分级采样器( KS30310/2.5/1.0),总悬浮颗粒物 (total suspended particles,TSP)采样器和粒径小于 10 μm的颗粒物(PM10)采 样器。研究结果表明,分级采样器和 TSP采样器所监测到的 PCNs和 PCBs的浓 度具有可比对性(PCNs:R2 = 0.978;PCBs:R2 = 0.974,p < 0.05),其同系物/同 类物具有相似的分布特征,均能较好地反映空气中 PCNs和 PCBs的分布。利用 TSP与PM10采样器所监测到的PCNs和PCBs浓度也具有较好的可比对性(PCNs:R2= 0.940;PCBs:R2 = 0.924,p < 0.05),同系物/同类物的分布特征也较为相似。 2、系统研究了大气中 PCNs和 PCBs的污染水平、气固相分配以及粒径分布 特征。利用大流量分级采样器(KS30310/2.5/1.0)在北京城市生态系统研究站采集 城区大气样品,结果显示∑PCNs和∑PCBs的浓度处于较低水平,均主要分布在 气相中。在空气动力学直径(aerodynamic diameter,dae)分别为 > 10 µm、2.5– 10 µm、1.0–2.5 µm和 ≤ 1.0 µm的四个不同粒径颗粒相组分中,大气颗粒物浓度、 PCNs和 PCBs的浓度均随颗粒物粒径的增大而减小,在 dae ≤ 1.0 μm的颗粒相组 分中含量最高。不同粒径颗粒相中的 PCNs同系物分布特征相似,但不同于气相 中的分布特征。而 PCBs无论是在气相还是颗粒相中,tetra-CBs均是主要的贡献 同系物,其次是 tri-CBs。 雾霾重污染天气下,大气中 PCNs和 PCBs含量明显提高,分布特征发生一 定的变化。以非雾霾天为对照,结果显示雾霾天 PCNs和 PCBs的平均浓度 (∑PCNs:579 pg/m3 ;∑PCBs:39.2 pg/m3)明显高于非雾霾天(∑PCNs:221 pg/m3;∑PCBs:10.1 pg/m3)。雾霾天 PCNs和 PCBs的分布特征明显不同于非雾霾天,雾霾天颗粒相中高氯代同系物的贡献明显增加。此外,气固相分配机理研究表明, 雾霾天颗粒物中 PCBs是以吸附在颗粒物表面为主,非雾霾天则结合到颗粒物的 有机质中。 3、研究了再生铜冶炼厂车间空气中 PCNs和 PCBs的污染水平与粒径分布 特征,结果表明其倾向于存在更小粒径颗粒物中(dae ≤ 1.0 μm)。利用大流量分 级采样器(KS30310/2.5/1.0)采集了两家典型再生铜冶炼厂的车间空气,分析车间 空气中 PCNs和 PCBs的污染水平及其在不同粒径颗粒物上的分布特征。结果表 明,两家再生铜冶炼厂车间空气中的 PCNs和 PCBs浓度相当,气固相分配特征 相似,均为低氯代同系物主要存在于气相中,在不同粒径颗粒物上的浓度均随着 粒径的增大而减少。归一化的粒径分布特征结果表明,车间空气中 PCNs和 PCBs 主要存在于更小粒径的颗粒物中,与环境空气明显不同。
英文摘要: Polychlorinated naphthalenes (PCNs) and polychlorinated biphenyls (PCBs) are persistent organic pollutants with similar structures and properties. Because they are highly toxic, persistent, and accumulate in the environment, they pose potential risks to human health and the environment. Atmosphere is a major medium for the transport and deposition of PCNs and PCBs, and it is also one of direct pathways for human exposure. In recent years, many studies have been conducted on the levels, environmental behavior, and potential sources of PCNs and PCBs in the air. However, it is difficult to compare data for airborne PCNs and PCBs because of the different sampling methods used. To date, studies have focused on gas phase PCNs, and gas- particle partitioning and particle size distributions of PCNs are still unclear. Therefore, comprehensive studies of the levels, gas-particle partitioning, and size distributions of PCNs and PCBs in the air are required. This will increase understanding of their environmental behavior, and could be used to assess human exposure via inhalation. In this study, sampling methods for airborne PCNs and PCBs were compared. The levels, gas-particle partitioning, and size distribution were investigated for PCNs and PCBs in the ambient air and workplace air. The major aspects of this study are detailed below. 1. High volume air samplers (cascade impactor, total suspended particulate (TSP) sampler, and PM10 sampler) were used to collect air samples at the Beijing urban ecosystem research station. The PCN and PCB concentrations obtained using the cascade impactor (KS30310/2.5/1.0) and TSP sampler were comparable (PCNs: R2 = 0.940; PCBs: R2 = 0.924, p < 0.05) and the homolog/congener profiles were similar. These results suggest that both these air samplers can be used to study the distributions of PCNs and PCBs in air. The concentrations of PCNs and PCBs in air collected by the TSP and PM10 samplers were also similar (PCNs: R2 = 0.940; PCBs: R2 = 0.924, p < 0.05). 2. The levels, gas-particle partitioning and size distributions of PCNs and PCBs in ambient air were determined using the cascade impactor (KS30310/2.5/1.0). The concentrations of PCNs and PCBs were relatively low in the atmosphere. Most of the PCNs and PCBs were in the gas phase. The concentrations of particulate matter (PM), PCNs, and PCBs increased as the particle size decreased (dae > 10 µm, 2.5–10 µm, 1.0– 2.5 µm and dae ≤ 1.0 µm). The highest concentrations were found in the dae ≤ 1.0 µm PM fraction. The homolog profiles of PCNs in different PM fractions were similar, but different to those in the gas phase. However, the PCB profiles were similar in the gas phase and PM fractions, with the dominant homolog being tetra-CBs, followed by tri- CBs. The influence of the concentrations and distributions of airborne PCBs during haze days was also explored in this study. The concentrations of PCNs and PCBs during haze days (∑PCNs:579 pg/m3 ;∑PCBs:39.2 pg/m 3) were obviously higher than those The profiles of PCNs during normal days (∑PCNs:221 pg/m3;∑PCBs:10.1 pg/m3 and PCBs ).during haze days were different from those during normal days. In addition,PCBs were mainly adsorbed on the surface of particles during haze days, whereas during normal days they were primarily absorbed into the particles. 3. The concentrations and size distributions were assessed for PCNs and PCBs in the workplace air from two secondary copper smelters collected with the cascade impactor (KS30310/2.5/1.0). The concentrations of PCNs and PCBs in the workplace air of the two secondary copper smelters were comparable. The gas–particle partitioning was also similar, with lower chlorinated homologs mianly in the gas phase. The concentrations increased as the particle size decreased. However, the PCNs and PCBs tended to be associated with smaller particles (dae ≤ 1.0 μm), which was different to what we observed in the urban air.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38763
Appears in Collections:环境化学与生态毒理学国家重点实验室_学位论文

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作者单位: 1.中国科学院生态环境研究中心

Recommended Citation:
朱青青. 空气中多氯萘和多氯联苯的分布特征研究[D]. 北京. 中国科学院大学. 2017.
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