印刷电路板生产、回收拆解及废弃堆置过程中重金属与溴系阻燃剂的污染、释放规律及人体暴露研究
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摘要
印刷电路板(PCB)是所有电子电气产品(EEE)中重要的基础部件之一。我国作为全球最大的PCB生产基地,每年的产量可达21400万平方米。在PCB的生产、回收拆解及废弃堆置过程中会产生并释放出大量的污染物,其中包括重金属与溴系阻燃剂(BFRs)。然而,已有的研究比较零散,尚未针对PCB整个产品生命周期过程中重金属与BFRs的污染与释放规律进行综合性的研究,亦未评估对PCB生产、回收从业人员人体健康的潜在影响。
本研究在建立了多种环境介质与固体废弃物样品中重金属(Cu、Zn、Pb、Ni、Cd、 Cr、Sn)以及多溴联苯醚(PBDEs)、四溴双酚A (TBBPA)分析检测方法的基础上,首先调查了PCB中污染物质的含量与普遍赋存特征,而后针对PCB生命周期中三个重要阶段(1)生产、(2)回收拆解以及(3)废弃处置过程,通过现场采样调查与实验室模拟实验相结合的方法,系统考察了上述三个过程中重金属与BFRs在生产车间、回收单元以及模拟填埋环境中的污染情况,阐释了污染物的分布特征与释放规律,并且评估了污染物的人体暴露与健康风险。主要结果和结论如下：
首先,从我国典型电子垃圾(WEEE)拆解区、有资质的VEEE资源化再生利用企业以及小型废旧家电回收点等处采集了具有代表性的废弃电路板(WPCB)样品(n92),经过分析发现各重金属含量由高到低为：Cu(189g/kg)>Sn(33.0g/kg)>Pb(17.1g/kg)>Zn(8.91g/kg)>Ni(1.93g/kg)>PBDEs(0.79g/kg)>Cr(0.44g/kg)>Cd(0.26g/kg)>TBBPA(0.17g/kg),其中Pb、Cd超过了RoHS指令规定的限值。PBDEs同系物的指纹图谱与Penta-BDE工业品相似程度较高,BDE-47与BDE-99所占比例最大,表明WPCB与废塑料等WEEE不同,采用Penta-BDE工业品作为主要添加剂,是环境中低溴代联苯醚污染的直接来源之一；将WPCB样品根据不同产品、年代、地区进行分类,发现其所含污染物存在较大差异,其中1995-2000年问来自中国和日本电视机的WPCB污染最严重,有效地分选出高污染WPCB能够更好地控制BFRs的潜在释放与环境污染。采用物质流分析法(SFA)对国内WPCB中重金属与BFRs的赋存量进行了推算,至2010年底,我国WPCB中(Cu、Zn、Pb、Ni、Cd、Cr、Sn、PBDEs和TBBPA的赋存量分别为338000、13700、6010、3300、300、31300、429和40.6吨。此外研究发现2006年后Pb、Cr和PBDEs等RoHS限制物质的累积赋存量的增长趋势减缓,PBDEs的增长率从30%-40%下降到了6%左右,说明RoHHS指令的实施有效地抑制了EEE中有毒有害物质的使用。
其次,对PCB生产过程的污染及其释放特征进行了研究,同时评估从业工人的人体暴露风险。通过对典型PCB生产厂家生产废料(废粉料、清洗废水、污水处理设施脱水污泥与最终出水)进行分析,研究发现Cu、Zn、Pb、Ni、Cr、Sn以及TBBPA污染普遍存在,而Cd与PBDEs均未检出,表明减少RoHS限制物质的使用己成为了PCB生产的主流趋势；最终出水中污染物的含量均处于较低水平,TBBPA浓度甚至低于我国湖泊水,表明良好地管理PCB生产活动将有助于控制其对自然水体造成的污染。生产废料中污染物的释放系数呈现以下规律：Cu>Zn>Sn≈Ni>Pb>Cr>>TBBPA,消耗清洗废水的“湿制程”是重金属污染的主要来源,而产生废粉料的“干制程”则是TBBPA污染的源头。此外,Cu向水体和土壤的年均释放总量分别达到了11400和1910kg；TBBPA的释放仅为0.02和<0.01kg,因此可以忽略TBBPA对环境造成的负面影响。
随后,分析了采集自PCB生产车间的灰尘与PM1o样品,结果显示,重金属与TBBPA含量均高于文献报道同类场所的参考值。PM10样品中不同重金属之间相关性较好,表明存在相同的污染来源,扫描电镜显示了PM1o由环氧树脂颗粒、玻璃纤维束以及自然颗粒物组成,说明了生产过程废粉料是污染的重要来源；灰尘样品中重金属之间的相关性较差,其污染来源较为复杂。利用灰尘和PM1o中污染物浓度之比的对数Log (dust/PM10)值表征了污染物在两相间的分配规律。重金属的Log (dust/PM10)<0,污染以PM1o颗粒相为主；TBBPA的Log (dust/PM10)>0,表明灰尘是TBBPA污染的重要载体。根据不同车间Log(dust/PM10)值的谱系聚类分析显示,污染物的分配规律存在3种情况,主要由车间所涉及的生产工艺决定。
对车间内污染物人体暴露量的贡献进行了估算,依次是Cu(73.4%)>Sn(10.0%)>Zn(9.38%)>Cr(3.61%)>Pb(2.15%)>Ni(1.09%)。TBBPA的暴露量远低于重金属,但高于国内外文献报道的的平均值,因此PCB生产是导致职业环境中TBBPA暴露的重要途径之一。灰尘摄入是从业工人主要暴露途径,占总暴露量69.5%-96.9%。单个重金属的非致癌风险HI均小于1,基本不会对从业工人人体健康造成危害；而5种重金属HI的总和在捞边车间中大于1,表明多种重金属非致癌风险的累积可能会对从业工人的人体健康造成一定的危害。Cr的Risk值在致癌风险阈值范围之内,Cr存在一定的致癌风险。
再次,针对WPCB回收拆解过程的污染特征与暴露风险进行了研究。在一家典型的WEEE资源化再生利用企业中,研究发现WPCB手工预拆解车间内灰尘与PM10样品中的污染高于机械拆解车间。手工预拆解车间Pb的污染比较严重；而机械拆解车间受WPCB拆解影响,Cu为最主要的污染物。除Cu外,车问内重金属污染主要发生在PM10颗粒相中。车间环境样品中PBDEs同系物以BDE-209为主,与WPCB原材料中的组成不相符(BDE-47、BDE-99为主)。分析认为该现象主要由各PBDEs同系物在气相与颗粒相中分配能力的差异所致。此外,WPCB拆解车间还可能受到其他拆解行为的影响(拆解高BDE-209含量的塑料)。不同车间中污染物的HI均大于1,其中Pb的非致癌风险的“贡献”最大(84%),表明拆解工人在拆解活动中面临着一定的非致癌健康风险。致癌重金属Cr、Cd和Ni的Risk值均超过了致癌风险阈值范围,表明WPCB拆解过程存在一定的致癌风险,且大于PCB生产过程。
最后,分别采用了TCLP、SPLP以及NIES改进浸出法研究了模拟堆置条件下WPCB中重金属与BFRs的浸出特征。结果显示,WPCB所含重金属在标准TCLP、SPLP浸出法中的浸出浓度特征为Cu>Pb>Sn>Zn>Cr>Cd>Ni,其中Cu和Pb浸出毒性最大。BFRs在NIES改进浸出法中的浸出遵循一阶指数衰减方程,显示出先快速浸出而后缓慢趋向于浸出平衡的现象；浸提剂种类、目标污染物性质以及WPCB的比表面积等因素会对BFRs的浸出率产生影响；浸出液中PBDEs同系物的组成与实际垃圾填埋场渗滤液中低溴代联苯醚的组成相似；通过计算,2010年底我国填埋场中BFRs潜在浸出总量达到了101kg。因此,在随意丢弃、露天堆放或不规范填埋等不当处置情况下,WPCB所含BFRs将在短时间内浸出并对周边环境造成污染,是填埋地土壤、渗滤液甚至地下水中污染的重要来源。
Printed circuit board (PCB) is one of the essential components in all electric and electronic equipments (EEE). As the global PCB production base, China has the largest production amount which is estimated to be214million m. Hundred kinds of chemicals including heavy metals and brominated flame retardants (BFRs), are involved and released during the PCB production, recycling and disposal processes, which may cause severe environmental pollution. However, comprehensive study on contamination and emission of heavy metals and BFRs during the whole life cycle of PCB product is currently limited.
In this study, reliable analytical and instrumental methods were built up for the qualitative and quantitative determination of Cu, Zn, Pb, Ni, Cd, Cr, Sn, Polybrominated Diphenyl Ethers (PBDEs) and Tetrabromobisphenol A (TBBPA) in PCB, solid waste and environmental samples. Field investigation and laboratory simulation were both conducted to investigate the contamination and emission of heavy metals and BFRs in three important processes of life cycle of PCB as follows:(1) production,(2) recycling and (3) disposal. Meanwhile, the heavy metals and BFRs released to the environment and the human exposure to those substantces were also evaluated in the above processes.
A total of92representative waste printed circuit board (WPCB) samples were randomly collected from large e-waste recycling facilities and small dismantling workshops in China and analyzed for heavy metals and BFRs. The mean concentration exhibited the following order:Cu (189g/kg)> Sn (33.0g/kg)> Pb (17.1g/kg)> Zn (8.91g/kg)> Ni (1.93g/kg)> PBDEs (0.79g/kg)> Cr (0.44g/kg)> Cd (0.26g/kg)> TBBPA (0.17g/kg), with Pb and Cr exceeding the RoHS regulatory limits. The PBDEs profile in our samples of which BDE-47and BDE-99contributed to the majority were quite comparable with the Penta-BDE technical mixture. It suggested that the Penta-BDE techincal mixture used in WPCB, unlike the case of waste plastic, was one of the direct emission sources of lower-BDEs in the environment. Wide variations of the occurrences of heavy metals and BFRs were found in WPCB samples of different source, production place and date, indicating the WPCB from Chinese and Japanese TV sets produced in1995-2000were most highly polluted among all samples. Sorting of those materials is helpful for accomplishing a better control of the potential pollutant release in the subsequent disposal processes. Substance flow analysis was applied to estimate the pollutant inventories in WPCB and the results showed that the increasing tendency of the cumulative inventory of RoHS regulated substance, e.g., Pb, Cr and PBDEs, began to decline after2006, especially for PBDEs (dropping from30-40%to6%). It evidently showed the positive impact of RoHS direction on reducing the application of hazardous substance in EEE.
Cu, Zn, Pb, Ni, Cr, Sn and TBBPA were ubiquitous in production wastes collected from a typical PCB plant while Cd and PBDEs were not detected, which was in agreement with the phase-out of hazardous substance in EEE. The low pollutant levels in the effluent showed that limited pollution was released to the environment from well-managed PCB production. The emission factors of pollutants were caculated as follows:Cu> Zn> Sn≈Ni> Pb> Cr>> TBBPA. Emission of heavy metals and BFRs were mainly originated from wet process that consumed rinsing water and dry process that produced solid waste, respectively. Annual emission of Cu to water and land were estimated to be11400and1910kg and those of TBBPA were quite minor (0.02and<0.01kg), which had negligible impact on environment.
Heavy metals and BFRs levels in PM10and dust samples from PCB production workshop were relatively higher than those in other related locations ever reported in literatures. Significant correlation among heavy metal in PM10samples suggested similar emission sources. However, insignificant correlation in dust samples indicated that emission sources were more complicated for dust. The distribution of pollutant between dust and PM10were characterised by comparing their concentrations in two phases and the results were given in Log (dust/PM10). The heavy metals pollution occurred mainly in the form of PM10with Log (dust/PM10)<0. Contrarily, TBBPA pollution occurred in the form of dust with Log (dust/PM10)>0. According to the Ward's clustering method, the distribution pattern was categoried into3types, depending on the production process involved in the workshop.
The exposure contribution in workshop presented the following trend:Cu (73.4%)> Sn (10.0%)> Zn (9.38%)> Cr (3.61%)> Pb (2.15%)> Ni (1.09%). TBBPA exposure was quite minor compared to heavy metals but still much higher than the reported value in literature, which indicated that PCB production was an important occupational exposure source of BFRs. Dust ingestion contributed to the majority (69.5%-96.9%) of total exposure pathway. Total Hazardous Index (HI) values of heavy metal exceeded the acceptable level in the milling worshop which suggested potential noncancerous toxic risk to the workers. Carcinogenic risk value of Cr was greater than the threshold value of10"6, suggesting the potential cancerous risk to the worker.
Heavy metals and BFRs contamination during WPCB dismantling process was investigated based on a typical WEEE recycling facility. In general, dust and PM10samples from the manual pre-dismantling workshop contained higher levels of heavy metals than those from the mechanical dismantling workshop. Pb was the predominate element in the samples from manual pre-dismantling workshop, whlie the mechanical dismantling workshop was mainly polluted by Cu, resulting from the WPCB dismantling activities. The heavy metals pollution occurred mainly in the form of PM10in the dismantling workshop, which was similar to the PCB production. BDE-209was the predominate congener in the environmental samples collected from WPCB dismantling workshop, which was in disagreement with the congener profile in the WPCB material that was predominated by BDE-47and BDE-99. It was mainly attributed to the vapor/particle partitioning of PBDE congeners in ambient air. In addition, the WPCB dismantling workshop might also be influenced by the dismantling activities of other WEEE, such as plastic that contained high concentration of BDE-209. HI values in both dismantling workshops exceeded the acceptable level, which indicated the potential noncancerous toxic risk to the dismantling workers. Carcinogenic risk value of Ni, Cr and were greater than the threshold value of10-6, which suggested that the workers were exposed to the cancerous risk caused by the dismantling of WPCB.
Leaching tests of WPCB using TCLP and SPLP showed the leaching concentration of Cu> Pb> Sn> Zn> Cr> Cd> Ni, with Cu and Pb being the most leachable elements. In the modified NIES leaching tests, initially leacing concentration of BFRs increased sharply, then maintained or even slightly declined after a certain contact period. The leaching behavior fitted well with first-order exponential decay equation and the leaching ratio was influenced by the leachate, the target substance and the specific surface area of WPCB. The potential leached-out volume of BFRs in domestic landfill sites was estimated to reach101kg by the end of2010. These results showed that BFRs had the potential to leach out in short period and became pollution source to soil, landfill leachate and even underground water ocne WPCB were discarded, dumped or disposed in improper ways.
本研究在建立了多种环境介质与固体废弃物样品中重金属(Cu、Zn、Pb、Ni、Cd、 Cr、Sn)以及多溴联苯醚(PBDEs)、四溴双酚A (TBBPA)分析检测方法的基础上,首先调查了PCB中污染物质的含量与普遍赋存特征,而后针对PCB生命周期中三个重要阶段(1)生产、(2)回收拆解以及(3)废弃处置过程,通过现场采样调查与实验室模拟实验相结合的方法,系统考察了上述三个过程中重金属与BFRs在生产车间、回收单元以及模拟填埋环境中的污染情况,阐释了污染物的分布特征与释放规律,并且评估了污染物的人体暴露与健康风险。主要结果和结论如下：
首先,从我国典型电子垃圾(WEEE)拆解区、有资质的VEEE资源化再生利用企业以及小型废旧家电回收点等处采集了具有代表性的废弃电路板(WPCB)样品(n92),经过分析发现各重金属含量由高到低为：Cu(189g/kg)>Sn(33.0g/kg)>Pb(17.1g/kg)>Zn(8.91g/kg)>Ni(1.93g/kg)>PBDEs(0.79g/kg)>Cr(0.44g/kg)>Cd(0.26g/kg)>TBBPA(0.17g/kg),其中Pb、Cd超过了RoHS指令规定的限值。PBDEs同系物的指纹图谱与Penta-BDE工业品相似程度较高,BDE-47与BDE-99所占比例最大,表明WPCB与废塑料等WEEE不同,采用Penta-BDE工业品作为主要添加剂,是环境中低溴代联苯醚污染的直接来源之一；将WPCB样品根据不同产品、年代、地区进行分类,发现其所含污染物存在较大差异,其中1995-2000年问来自中国和日本电视机的WPCB污染最严重,有效地分选出高污染WPCB能够更好地控制BFRs的潜在释放与环境污染。采用物质流分析法(SFA)对国内WPCB中重金属与BFRs的赋存量进行了推算,至2010年底,我国WPCB中(Cu、Zn、Pb、Ni、Cd、Cr、Sn、PBDEs和TBBPA的赋存量分别为338000、13700、6010、3300、300、31300、429和40.6吨。此外研究发现2006年后Pb、Cr和PBDEs等RoHS限制物质的累积赋存量的增长趋势减缓,PBDEs的增长率从30%-40%下降到了6%左右,说明RoHHS指令的实施有效地抑制了EEE中有毒有害物质的使用。
其次,对PCB生产过程的污染及其释放特征进行了研究,同时评估从业工人的人体暴露风险。通过对典型PCB生产厂家生产废料(废粉料、清洗废水、污水处理设施脱水污泥与最终出水)进行分析,研究发现Cu、Zn、Pb、Ni、Cr、Sn以及TBBPA污染普遍存在,而Cd与PBDEs均未检出,表明减少RoHS限制物质的使用己成为了PCB生产的主流趋势；最终出水中污染物的含量均处于较低水平,TBBPA浓度甚至低于我国湖泊水,表明良好地管理PCB生产活动将有助于控制其对自然水体造成的污染。生产废料中污染物的释放系数呈现以下规律：Cu>Zn>Sn≈Ni>Pb>Cr>>TBBPA,消耗清洗废水的“湿制程”是重金属污染的主要来源,而产生废粉料的“干制程”则是TBBPA污染的源头。此外,Cu向水体和土壤的年均释放总量分别达到了11400和1910kg；TBBPA的释放仅为0.02和<0.01kg,因此可以忽略TBBPA对环境造成的负面影响。
随后,分析了采集自PCB生产车间的灰尘与PM1o样品,结果显示,重金属与TBBPA含量均高于文献报道同类场所的参考值。PM10样品中不同重金属之间相关性较好,表明存在相同的污染来源,扫描电镜显示了PM1o由环氧树脂颗粒、玻璃纤维束以及自然颗粒物组成,说明了生产过程废粉料是污染的重要来源；灰尘样品中重金属之间的相关性较差,其污染来源较为复杂。利用灰尘和PM1o中污染物浓度之比的对数Log (dust/PM10)值表征了污染物在两相间的分配规律。重金属的Log (dust/PM10)<0,污染以PM1o颗粒相为主；TBBPA的Log (dust/PM10)>0,表明灰尘是TBBPA污染的重要载体。根据不同车间Log(dust/PM10)值的谱系聚类分析显示,污染物的分配规律存在3种情况,主要由车间所涉及的生产工艺决定。
对车间内污染物人体暴露量的贡献进行了估算,依次是Cu(73.4%)>Sn(10.0%)>Zn(9.38%)>Cr(3.61%)>Pb(2.15%)>Ni(1.09%)。TBBPA的暴露量远低于重金属,但高于国内外文献报道的的平均值,因此PCB生产是导致职业环境中TBBPA暴露的重要途径之一。灰尘摄入是从业工人主要暴露途径,占总暴露量69.5%-96.9%。单个重金属的非致癌风险HI均小于1,基本不会对从业工人人体健康造成危害；而5种重金属HI的总和在捞边车间中大于1,表明多种重金属非致癌风险的累积可能会对从业工人的人体健康造成一定的危害。Cr的Risk值在致癌风险阈值范围之内,Cr存在一定的致癌风险。
再次,针对WPCB回收拆解过程的污染特征与暴露风险进行了研究。在一家典型的WEEE资源化再生利用企业中,研究发现WPCB手工预拆解车间内灰尘与PM10样品中的污染高于机械拆解车间。手工预拆解车间Pb的污染比较严重；而机械拆解车间受WPCB拆解影响,Cu为最主要的污染物。除Cu外,车问内重金属污染主要发生在PM10颗粒相中。车间环境样品中PBDEs同系物以BDE-209为主,与WPCB原材料中的组成不相符(BDE-47、BDE-99为主)。分析认为该现象主要由各PBDEs同系物在气相与颗粒相中分配能力的差异所致。此外,WPCB拆解车间还可能受到其他拆解行为的影响(拆解高BDE-209含量的塑料)。不同车间中污染物的HI均大于1,其中Pb的非致癌风险的“贡献”最大(84%),表明拆解工人在拆解活动中面临着一定的非致癌健康风险。致癌重金属Cr、Cd和Ni的Risk值均超过了致癌风险阈值范围,表明WPCB拆解过程存在一定的致癌风险,且大于PCB生产过程。
最后,分别采用了TCLP、SPLP以及NIES改进浸出法研究了模拟堆置条件下WPCB中重金属与BFRs的浸出特征。结果显示,WPCB所含重金属在标准TCLP、SPLP浸出法中的浸出浓度特征为Cu>Pb>Sn>Zn>Cr>Cd>Ni,其中Cu和Pb浸出毒性最大。BFRs在NIES改进浸出法中的浸出遵循一阶指数衰减方程,显示出先快速浸出而后缓慢趋向于浸出平衡的现象；浸提剂种类、目标污染物性质以及WPCB的比表面积等因素会对BFRs的浸出率产生影响；浸出液中PBDEs同系物的组成与实际垃圾填埋场渗滤液中低溴代联苯醚的组成相似；通过计算,2010年底我国填埋场中BFRs潜在浸出总量达到了101kg。因此,在随意丢弃、露天堆放或不规范填埋等不当处置情况下,WPCB所含BFRs将在短时间内浸出并对周边环境造成污染,是填埋地土壤、渗滤液甚至地下水中污染的重要来源。
Printed circuit board (PCB) is one of the essential components in all electric and electronic equipments (EEE). As the global PCB production base, China has the largest production amount which is estimated to be214million m. Hundred kinds of chemicals including heavy metals and brominated flame retardants (BFRs), are involved and released during the PCB production, recycling and disposal processes, which may cause severe environmental pollution. However, comprehensive study on contamination and emission of heavy metals and BFRs during the whole life cycle of PCB product is currently limited.
In this study, reliable analytical and instrumental methods were built up for the qualitative and quantitative determination of Cu, Zn, Pb, Ni, Cd, Cr, Sn, Polybrominated Diphenyl Ethers (PBDEs) and Tetrabromobisphenol A (TBBPA) in PCB, solid waste and environmental samples. Field investigation and laboratory simulation were both conducted to investigate the contamination and emission of heavy metals and BFRs in three important processes of life cycle of PCB as follows:(1) production,(2) recycling and (3) disposal. Meanwhile, the heavy metals and BFRs released to the environment and the human exposure to those substantces were also evaluated in the above processes.
A total of92representative waste printed circuit board (WPCB) samples were randomly collected from large e-waste recycling facilities and small dismantling workshops in China and analyzed for heavy metals and BFRs. The mean concentration exhibited the following order:Cu (189g/kg)> Sn (33.0g/kg)> Pb (17.1g/kg)> Zn (8.91g/kg)> Ni (1.93g/kg)> PBDEs (0.79g/kg)> Cr (0.44g/kg)> Cd (0.26g/kg)> TBBPA (0.17g/kg), with Pb and Cr exceeding the RoHS regulatory limits. The PBDEs profile in our samples of which BDE-47and BDE-99contributed to the majority were quite comparable with the Penta-BDE technical mixture. It suggested that the Penta-BDE techincal mixture used in WPCB, unlike the case of waste plastic, was one of the direct emission sources of lower-BDEs in the environment. Wide variations of the occurrences of heavy metals and BFRs were found in WPCB samples of different source, production place and date, indicating the WPCB from Chinese and Japanese TV sets produced in1995-2000were most highly polluted among all samples. Sorting of those materials is helpful for accomplishing a better control of the potential pollutant release in the subsequent disposal processes. Substance flow analysis was applied to estimate the pollutant inventories in WPCB and the results showed that the increasing tendency of the cumulative inventory of RoHS regulated substance, e.g., Pb, Cr and PBDEs, began to decline after2006, especially for PBDEs (dropping from30-40%to6%). It evidently showed the positive impact of RoHS direction on reducing the application of hazardous substance in EEE.
Cu, Zn, Pb, Ni, Cr, Sn and TBBPA were ubiquitous in production wastes collected from a typical PCB plant while Cd and PBDEs were not detected, which was in agreement with the phase-out of hazardous substance in EEE. The low pollutant levels in the effluent showed that limited pollution was released to the environment from well-managed PCB production. The emission factors of pollutants were caculated as follows:Cu> Zn> Sn≈Ni> Pb> Cr>> TBBPA. Emission of heavy metals and BFRs were mainly originated from wet process that consumed rinsing water and dry process that produced solid waste, respectively. Annual emission of Cu to water and land were estimated to be11400and1910kg and those of TBBPA were quite minor (0.02and<0.01kg), which had negligible impact on environment.
Heavy metals and BFRs levels in PM10and dust samples from PCB production workshop were relatively higher than those in other related locations ever reported in literatures. Significant correlation among heavy metal in PM10samples suggested similar emission sources. However, insignificant correlation in dust samples indicated that emission sources were more complicated for dust. The distribution of pollutant between dust and PM10were characterised by comparing their concentrations in two phases and the results were given in Log (dust/PM10). The heavy metals pollution occurred mainly in the form of PM10with Log (dust/PM10)<0. Contrarily, TBBPA pollution occurred in the form of dust with Log (dust/PM10)>0. According to the Ward's clustering method, the distribution pattern was categoried into3types, depending on the production process involved in the workshop.
The exposure contribution in workshop presented the following trend:Cu (73.4%)> Sn (10.0%)> Zn (9.38%)> Cr (3.61%)> Pb (2.15%)> Ni (1.09%). TBBPA exposure was quite minor compared to heavy metals but still much higher than the reported value in literature, which indicated that PCB production was an important occupational exposure source of BFRs. Dust ingestion contributed to the majority (69.5%-96.9%) of total exposure pathway. Total Hazardous Index (HI) values of heavy metal exceeded the acceptable level in the milling worshop which suggested potential noncancerous toxic risk to the workers. Carcinogenic risk value of Cr was greater than the threshold value of10"6, suggesting the potential cancerous risk to the worker.
Heavy metals and BFRs contamination during WPCB dismantling process was investigated based on a typical WEEE recycling facility. In general, dust and PM10samples from the manual pre-dismantling workshop contained higher levels of heavy metals than those from the mechanical dismantling workshop. Pb was the predominate element in the samples from manual pre-dismantling workshop, whlie the mechanical dismantling workshop was mainly polluted by Cu, resulting from the WPCB dismantling activities. The heavy metals pollution occurred mainly in the form of PM10in the dismantling workshop, which was similar to the PCB production. BDE-209was the predominate congener in the environmental samples collected from WPCB dismantling workshop, which was in disagreement with the congener profile in the WPCB material that was predominated by BDE-47and BDE-99. It was mainly attributed to the vapor/particle partitioning of PBDE congeners in ambient air. In addition, the WPCB dismantling workshop might also be influenced by the dismantling activities of other WEEE, such as plastic that contained high concentration of BDE-209. HI values in both dismantling workshops exceeded the acceptable level, which indicated the potential noncancerous toxic risk to the dismantling workers. Carcinogenic risk value of Ni, Cr and were greater than the threshold value of10-6, which suggested that the workers were exposed to the cancerous risk caused by the dismantling of WPCB.
Leaching tests of WPCB using TCLP and SPLP showed the leaching concentration of Cu> Pb> Sn> Zn> Cr> Cd> Ni, with Cu and Pb being the most leachable elements. In the modified NIES leaching tests, initially leacing concentration of BFRs increased sharply, then maintained or even slightly declined after a certain contact period. The leaching behavior fitted well with first-order exponential decay equation and the leaching ratio was influenced by the leachate, the target substance and the specific surface area of WPCB. The potential leached-out volume of BFRs in domestic landfill sites was estimated to reach101kg by the end of2010. These results showed that BFRs had the potential to leach out in short period and became pollution source to soil, landfill leachate and even underground water ocne WPCB were discarded, dumped or disposed in improper ways.
引文
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