珠江三角洲大气中卤代阻燃剂的污染特征、变化趋势及与PM_(2.5)的关系

Halogenated flame retardants in the atmosphere of the Pearl River Delta:Pollution characteristics, trends and relationship with PM_(2.5)

本研究采集了珠江三角洲9个城市的126对颗粒态(PM_(2.5))和气态大气样品,系统分析了8种多溴联苯醚(PBDEs)、6种新型溴代阻燃剂(NBFRs)和得克隆(DPs)等卤代阻燃剂,评估了其污染特征和历史变化趋势,探讨了卤代阻燃剂与PM_(2.5)的关系。结果表明,十溴二苯乙烷(DBDPE,中值浓度为59.91 pg/m^(3))是大气中浓度最高的阻燃剂,Σ_(7) PBDEs、十溴二苯醚(BDE-209)和Σ_(5) NBFRs(中值浓度分别为9.89 pg/m^(3)、8.37 pg/m^(3)和8.81 pg/m^(3))浓度相当,DPs(中值浓度为1.74 pg/m^(3))浓度最低。对比先前研究报道,可见包括BDE-209在内的PBDEs浓度显著下降,反映出区内限用、禁用PBDEs及电子垃圾管控的成效;DBDPE浓度则相对稳定。在颗粒相(PM_(2.5))中,部分溴代阻燃剂与PM_(2.5)浓度间呈现出相关性(如四溴邻苯二羧酸双(2-乙基己基)酯(TBPH)、Σ_(7) PBDEs),部分则无相关性(如BDE-209、DBDPE),可能是受到溴代阻燃剂理化性质、工业产品基体稳定性及其向大气排放途径等因素综合的影响。

In this study,126‘paired’particulate and gaseous atmospheric samples were collected from nine cities of the Pearl River Delta(PRD).The concentrations of eight polybrominated diphenylethers(PBDEs),six novel brominated flame retardants(NBFRs),and dechlorane plus(DPs)were systemically analyzed to evaluate their pollution characteristics and temporal trend.Furthermore,the relationship between levels of target compounds and PM_(2.5) was explored.Decabromodiphenyl ethane(DBDPE,median:59.9 pg/m^(3))was found to be the most abundant compound in the ambient air of PRD.Σ_(7) PBDEs,decabromodiphenyl ether(BDE-209)andΣ_(5) NBFRs(median 9.89,8.37 and 8.81 pg/m^(3),respectively)measured at similar atmospheric levels,whilst the concentrations of DPs(median 1.74 pg/m^(3))was at a lower range.Compared with previous studies,the concentration of PBDEs,including BDE-209,has decreased significantly,reflecting the effectiveness of restrictions and prohibitions of PBDEs and e-waste control in the PRD region.Meanwhile,the concentration of DBDPE was relatively stable.In the PM_(2.5) phase,several brominated flame retardants correlated with the PM_(2.5) concentration(such as bis(2-ethylhexyl)tetrabromophthalate(TBPH),Σ_(7) PBDEs),whereas some were not correlated(such as BDE-209,DBDPE).This could be due to the combined influence from the varied physicochemical property,matrix stability of commercial products,and emission pathway to the atmosphere of different halogenated flame retardants.