RCEES OpenIR  > 环境化学与生态毒理学国家重点实验室
京津冀大气中新型阻燃剂时空分布与人体呼吸暴露评价
Alternative TitleNovel flame retardants in the atmosphere of the Beijing Tianjin Hebei region: temporal spatial distribution and human respiratory exposure assessment
张巍巍
Subtype博士
Thesis Advisor张庆华
2019-06
Degree Grantor中国科学院生态环境研究中心
Place of Conferral北京
Degree Name理学博士
Degree Discipline环境科学
Keyword京津冀地区,大气,细颗粒物,有机磷酸酯,新型溴代阻燃剂 the Beijing Tianji n Hebei Region, Atmosphere, Fine Particle, o Rganophosphate Esters Novel b Rominated Flame Retardants
Abstract

      新型阻燃剂包括有机磷酸酯o rganophosphate esters, OPEs 和新型溴代阻燃剂 b rominate d flame retardants, NBFRs 等 因其 具有良好的阻燃性能 被大量应用在电子产品 、 纺织品 、 家具 、 建筑材料等领域。这些阻燃 剂主要以掺杂的方式添加,容易通过磨损 、 挥发 和 浸出等途径进入环境 。本研究选择人口密集,经济发展较快,同时大气污染问题突出的京津冀地区做为研究区域, 在该区域的典型城市 (北京、天津和石家庄)进行为期一 年( 2016 年 4 月 2017 年 3 月 )的样品收集 工作, 以此为基础 开展 新型阻燃剂在大气 环境 中的时空分布特征,气粒分配行为以及人体呼吸暴露 评价研究 为深入了解我国典型区域大气中典 型污染物的环境行为特征提供了科学依据 。 取得的主要研究结果如下:
      (1 )京津冀大气 (气相 颗粒相) 中 8 种 OPEs 总浓度( (∑ 8 OPEs )在 531 2180pg/m 3 范围内 。从年度均值来看, 天津 城区 OPEs 浓度水平最高。 季节分布 研究表明,夏季气相 中 OPEs 浓度水平较高,而冬季颗粒相 中 OPEs 浓度较高。温度和 相对湿度与 气相中 OPEs 的浓度呈显著的正相关关系 p < 0.05 )),而颗粒相中OPEs 的浓度 与 大气总悬浮颗粒物( TSP 高度相关 p < 0.01 。温度,相对湿度以及 TSP 浓度水平是影响 OPEs 季节和 区域分布的重要因素。气 粒分配行为研究表明,辛醇 气分配系数模型( K oa based model )的预测 结果 与实测值 较为一致,与 Junge Pankow 吸附分配模型 的预测值相比 具有更好 的拟合效果。
      (2 )京津冀大气中 9 种 NBFRs 的总浓度 ((∑ 9 NBFR s 在 1.65 344 pg/m 3范围内,年均值为 50 61 pg/m 3 。 其中 石家庄 城区的 浓度水平( 67 pg/m 3 )最高。DBDPE 是主要的化合物,占总浓度 70%70%,,∑ 8 NBFRs (除 DBDPE 外)在空间分布上与 ∑ 9 NBFRs 存在较大差异。总体来看, 冬 季 城市采样点的 ∑ 8 NBFRs 浓度水平相对较高,而 夏季 在郊区采样点 ∑ 8 NBFRs 的浓度水平较高。颗粒相中 NBFRs的浓度与 TSP 的浓度 高度相关 。与 OPEs 所 不同 的是 TSP 浓度 、 温度和大气边界层高度是影响大气中 NBFRs 时空分布的重要因素。 气 粒分配行为研究表明,NBFRs 中分子量较小的化合物 PBBz 、 PBT 、 PBEB 、 TBP DBPE 和 HBB 在气 粒分配 过程中受温度的影响较大。
      (3) 京津冀大气 PM 2.5 样品 中 ∑ 9 NBFRs 和 ∑ 8 OPEs 的浓度范围分别为 0.63-104 pg/m3 和 90 829 1 pg/m 3 。北京 地区 ∑ 9 NBFRs 和 ∑ 8 OPE s 浓度水平相对 较 高。人体呼吸 暴露评价 结果 表明, 儿童通过呼吸暴露 PM 2.5 中 NBFRs 的 剂量 高于成年人,儿童暴露 OPEs 的风险值是成人的 1.6 倍 ;相对于空气质量良好的天气重污染天气 人体 呼吸暴露 PM 2.5 中 OPEs 的风险 明显较高 。

Other Abstract

      Novel flame retardants (NFRs), which contain organophosphate esters (OP Es)and brominated flame retardants (NBFRs), are added to electronic equipment, textiles ,furniture, and building materials to prevent combustion and slow the spread of fire after ignition . Since NFR s are used as additives by mixing them into the materials ,rather than being chemically bonded, they could be leached out of the materials into ambient air via volatilization, dissolution, and abrasion. The B eijing T ianjin H ebei ( r egion is one of the most important city agglomerations in China . I n this regi on,rapid economic development and industrialization in the last several decades lead to serious environmental problems such as air pollution . T he air samples were collected from April 2016 to March 2017 at three repre s e n t a t i v e c i t i e s B e i j i n g T i a n j i n a n d S h i j i a z h u a n g a c r o s s t h e BTH r e g i o n In this study, the spatial and temporal distribution s of NFR s were investigate d in this metropolitan area. The gas/particle partitioning of NFR s was further explored and the inhalation exposure risk was also estimated based on the detected fine particle bound NFRs levels in the BTH Region. Th e main results of this research as below:
      (1)The mean atmospheric concentrations of ∑ 8 OPEs (gas and particle phases)varied from 531 ± 393 pg/m 3 to 2180 ± 1490 pg/m 3 with the highest levels observed at the urban sampling site in Tianjin City. Generally, h igher levels of gaseous OPEs were found in summer, while higher levels of particle bound OPEs were observed in winter. The concentrations of gaseous OPEs were positively and significantly correlated with local temperatures ( p < 0.05) and relative humidity p < 0.01), while significantly positive correlations were found between concentrations of particle bound OPEs and total suspended particulates (TSP) ( p < The result sconfirmed that temperature s , relative humidity and levels of TSP are the main drivers for OPE distribution s in different seasons and areas. Gas/particle partitioning of OPEs was also investigated based on the absorption partitioning model (octanol air partitioning coefficient (K oa ) based model) and Junge Pankow adsorption partitioning model (J P model). K oa based model generally showed a better performance in comparison with the measured results.
      (2)The atmospheric concentration of ∑ 9 NBFR s (gas and particle ranged from 1.65 to 344 pg/m 3 (annual average: 50 61 pg/m 3 ). T he highest levels observed at the urban sampling site in Shijiazhuang City 67 pg/m 3 Individual NBFR s were predominated by Decabromodiphenylethane (DBDPE), which accounted 70% of the ∑ 9 NBFR s concentrations across the BTH region. The spatial distribution of ∑ 8 NBFRs (except DBDPE) was different from that of ∑ 9 NBFR s . G enerally, relatively higher levels of ∑ 8 NBFRs were observed in winter months at urban sampling sites, while relatively higher levels of ∑ 8 NBFRs were observed in summer months at rural sampling sites. T he concentrations of TSP, temperature and the height of atmospheric boundary layer were key factors of influencing temporal distribution of ∑ 8 NBFRs. It was found that the gas particle partirioning coefficient for most low molecular weight NBFRs were highly temperature dependent
      (3)The concentration of ∑ 9 NBFR s were in the range of 0.63 104 pg/m 3 , while the levels of ∑ 8 OPEs ranged from 90 to 8291 pg/m 3 in atmospheric fine particle.Relatively higher levels of N FRs were found at urban sampling sites in Beijing City.Daily human exposure via inhalation revealed that children have a higher probability of suffering from the adverse effects of N FRs than tha t of adults. The hazard quotient values for children were ~ 1.6 times higher than those for adults. A higher health risk induced by fine particle bound OPEs via inhalation was estimated in severe haze days than in clear days.
 

Pages131
Language中文
Document Type学位论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/42350
Collection环境化学与生态毒理学国家重点实验室
Recommended Citation
GB/T 7714
张巍巍. 京津冀大气中新型阻燃剂时空分布与人体呼吸暴露评价[D]. 北京. 中国科学院生态环境研究中心,2019.
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