【作者】 陈来国；

【导师】 傅家谟； 麦碧娴； 冉勇；

【作者基本信息】 中国科学院研究生院（广州地球化学研究所） ， 环境科学， 2006， 博士

【摘要】 多溴联苯醚（PBDEs）是一类添加型的阻燃剂,广泛用于商业和家庭用品中,由于理化性质和多种其它的持久性有机污染物相似,它们已经成为无处不在的环境污染物,研究发现,在过去二十年,随着其它典型的持久性有机污染物（POPs,如PCBs）在环境中含量水平的下降,PBDEs在环境中的含量则呈现增加趋势,而国内还未见有关大气中PBDEs的研究.直至现在人们认为人体对PBDEs暴露的主要途径是通过食物途径,对室外大气和室内空气的研究相对较少,但最近的研究表明通过呼吸和室内尘土的摄入也是非常重要的途径,PCBs是环境中另一类重要的持久性有机污染物,但国内研究工作主要集中在对沉积物和土壤中PCBs进行研究,关于大气中PCBs的研究非常少。 本研究利用传统的大流量采样技术,对广州市区室外大气和室内空气环境中PBDEs和PCBs的浓度、组成、在气相/颗粒相中的分布和人体暴露水平、在不同粒径颗粒物上的分布特点及可能的控制因素进行了初步研究。 本研究初步获得以下主要结论: （1） 广州市区室外大气环境中∑₁₀PBDEs（BDE-28,-47,-66,-100,-99,-85,-154,-153,-138,-183）的含量范围为40-6600 pg/m³,除工业区附近的采样点外,污染程度与世界其它城市相当,而十溴联苯醚（BDE-209）的含量为100-15000 pg/m³,污染程度较重。工业区排放是市区大气中PBDEs污染的重要来源之一,无论在室外还是室内空气中,BDE-47、-99和BDE-209是最主要的成分,表明大气中PBDEs污染主要来自十溴联苯醚和五溴联苯醚工业品。 （2） 室外大气中PBDEs在气体-颗粒两相间的分配研究表明:城市中心区两相间的PBDEs分配趋向平衡。用Junge-Pankow的吸附模型和K_OA吸收模型的预测值和实测值进行了对比,结果表明K_OA吸收模型更好符合实测结果。 （3） 广州市区室内环境（家庭和工作环境）中∑₁₀PBDEs含量为120-8300 pg/m³,和国外研究结果相当。低溴的PBDEs（BDE-28,-47,-66）在部分室内环境中主要受室内排放源的影响,而另一部分室内环境则主要受室外影响;而高溴的PBDEs（BDE-138,-183,-209）主要受室外影响,在室内排放源中,电子电器类产品可能是主要的排放源,而含海绵的家俱类产品排放可能是次要的。更多还原

【Abstract】 Polybrominated diphenyl ethers(PBDEs) are a group of additive flame retardants widely used in commercial and household products. They have been recognized as ubiquitous environmental pollutants due to their similarity in physicochemical properties to a number of other persistent organic pollutants (POPs). In the past of 20 years, in contrast to the decreasing levels of most POPs, PBDEs levels in the environment are increasing. In China, report on PBDEs in atmosphere is blank. Polychlorinated biphenyls (PCBs) are else a group of all-known environmental pollutants. In China, the studies on PCBs have focused on the sediments and soil, however, research on atmospheric PCBs is nearly blank. Up to now, human exposure assessment to PBDEs has largely focused on the dietary pathway, few studies have examined exposure via inhalation or the other oral conduits such as dust, soil. However, recent studies imply that the pathways via inhalation and home dust intake are important human exposure pathways for PBDEs.This study reported PBDEs and PCBs concentrations, compositions, distributions, gas/particle two phases partitioning in outdoor and indoor air in Guangzhou, moreover, also reported human inhalation exposure for PBDEs and the distributions in different size particles and possible affecting factor.From this study, the following conclusions can be drawn:1. ∑ 10PBDEs concentrations in the atmosphere of Guangzhou(BDE-28, -47, -66, -100, -99, -85, -154, -153, -138, -183) ranged from 40 to 6600 pg/m~3 and were comparative with other cities of the world, however, BDE-209 concentrations (100-15000 pg/m~3) were higher than those cities. The industrial zone was a major emission source for urban PBDEs pollution. BDE-47, -99 and BDE-209 were dominated components in detected ∑ 11PBDEs in indoor and outdoor air, implying that in atmosphere of Guangzhou PBDEs primarily came from deca-BDE and penta-BDE commercial mixtures.2. The study on PBDEs gas/particle phases partitioning indicated: PBDEs appeared to be closer to equilibrium gas/particle phases at urban center than other samplingsites. The predicted values of two models (Junge-Pankow adsorption model and Koa absorption model) were compared with the measured values in the atmosphere of Guangzhou, the results indicated that the Koa absorption model worked better than the Junge-Pankow adsorption model.3f The ￡ ioPBDEs concentrations in indoor environments(home and workplace) of Guangzhou ranged from 120 to 8300 pg/m3 and were comparative with relative foreign studies. For low brominates PBDEs(i.e. -28, -47, -66) indoor air primarily was effected by the indoor emission sources in some indoor environments and by outdoor air in the other. However, those high brominates PBDEs(i.e. -138, -183, -209) predominantly came from infiltration of outdoor particle. In indoor emission sources, electronic/electrical products may be major emission sources, while the contributor from containing-PUF furniture was small. The median ￡ ioPBDEs exposure value for adults was 11.9 ng/day/person, higher than two relative studies.4. From individual PBDE distribution in six different stage size aerosol particles, BDE-47, -66, -100 and -99 were similar each other and primarily distributed in fine particles. The similarity with "saddle" symmetry was between BDE-208 and -207, but their distributions are different from BDE-47, -66, -99, -100. BDE-209 distribution was different from above two kinds of types, primarily distributed in coarse particles. Good linear relationships were found out between TC and BDE-28, -47, -100, -99, while poor correlation coefficients were between BDE-207, -208, -209 and TC, this difference may reflect different manner entering atmosphere or partitioning velocity in gas/particle of individual congener.5. E 64PCBs concentrations in the outdoor air of Guangzhou ranged from 160 to 2720 pg/m3, similar to most of relative studies in north America, Europe and Asia. Compared with ￡ioPBDEs(excluding BDE-209), X64PCBS concentrations were approximately a factor of 2-3 higher than ￡ ioPBDEs excluding sampling site near industrial zone, suggesting urban center and old industrial district were obvious emission sources for PCBs. The tri- and tetra-chlorinated biphenyls were the most abundant homologue groups in this study and consistent with most relative research. However, the individual congener distribution was different from other studies dueto different industrial products used in China.更多还原