印刷电路板生产企业多溴联苯醚和重金属污染排放特征以及对典型区域环境的影响研究
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摘要
印刷电路板(Printed Circuit Boards, PCB)是当代电子元件中最为活跃的产业,据中国电子元件行业协会印刷电路分会的调查,2003年中国印刷电路板的生产产值为500.69亿元,同比增长32.4%,超过美国,次于日本,居世界第二位。与此同时,由于印刷电路板生产过程中产生的废水、固体废弃物中含有重金属和PBDEs,日本和韩国很多企业搬入我国各个城市,使我国的重金属和PBDEs污染趋势加剧。印刷电路板产业虽然并未列入重污染行业,但作为相对耗水、耗能较多,同时又是污染排放物较多的产业,值得我们关注。PCB制造企业的污染主要产生在钻孔、蚀刻、电镀、金属化、去膜、显影等工艺过程中,排放的污染因子主要是工业废水,其次是固体废弃物。但以往的研究更多的是关注废水和固定废弃物中重金属的污染问题,对于钻孔、蚀刻过程中PBDEs的污染问题关注较少。因此,本文的主要研究内容就是印刷电路板生产企业PBDEs和重金属污染排放特征以及对典型区域环境的影响。
在实验室建立可靠的环境介质中PBDEs和重金属分析检测方法的基础上,通过前期的文献调研、印刷电路板生产企业联系和实地考察,选择了具有代表性的印刷电路板生产企业为我们的主要研究对象。然后,系统采集印刷电路板各生产流程、车间的原料、清洗水、灰尘和大气样品。通过分析得出印刷电路板生产原料中含有不同浓度的重金属,其中Cu的含量最高,在28000-438000mg/kg之间,其他重金属的浓度比Cu低几个数量级,浓度由高低分别是Zn>Pb>Ni>Cd；原料中几乎没有PBDEs。而在其生产过程中产生的污水和污泥中,也检测到了不同浓度的重金属和PBDEs。出水样品中检测出的含量最高的重金属是Cu(1.14±0.71mg/L),接着是Pb(0.09±0.03mg/L),Ni(0.04±0.01mg/L)和Cd(N.D.),而几乎不含有PBDEs;污泥中重金属浓度最高的是Cu,浓度为(1.71±0.49)×105(mg/kg dw),接下来分别是Ni(1640.36±484.77mg/kg dw)、Pb(791.63±112.05mg/kg dw)和Cd(ND),PBDEs浓度为0.02±0.01ng/kg dw。印刷电路板在生产过程中会产生大量的悬浮颗粒物,各车间空气中TSP、PM1o和PM2.5浓度分别在6.1-365.3、27.1-289.8和22.1-212.3μg/m3之间；各车间大气中PM1o和TSP以及PM2.5和PM1o之间的相关性都非常好,而且PM2.5所占比例在50%-80%之间；说明车间大气颗粒物来源一致,另外车间除尘装置对车间空气中颗粒物有很好的去除效果。各车间大气TSP、PM1o和PM2.5中Zn的浓度是最高的,其他金属浓度由高到低依次是Cu>Pb≈Cr>Ni>Cd。
印刷电路企业各车间灰尘样品的粒径范围在0.3-750μm之间。其中PM2.5和PM1o所占百分比分别在5.59-10.72%和14.22-26.15%之间。各个车间灰尘样品的体积平均直径D(4,3)从大到小依次为：钻孔车间(47.83gm)>原料仓库(44.11μm)>压合车间(41.53μm)>成型车间(37.371μm)>捞边车间(32.76μm)>下料车间(31.23μm)。灰尘中浓度最高的重金属是Cu,其浓度范围为6.54-56.31mg/g；其他金属浓度由高到低依次是Zn、Pb、Cr、Ni和Cd,其浓度范围分别为0.77-4.47,0.26-0.49,0.39-1.59,0.13-0.41和nd-0.056mg/g。各采样点的灰尘中均没有检出低溴代的BDEs,而只检测出少量的BDE-209。而就TBBPA来说,各车间的浓度差异较大,浓度在125-9091ng/g之间。另外,类似于RoHHS指令一样的相关法令对部分重金属(Pb)和溴系阻燃剂在印刷电路板生产工艺中的使用有决定性的影响。通过灰尘和空气颗粒物中重金属的浓度和相关风险评价模型对各车间进行风险评价发现：就各重金属的非致癌性风险来说,不管是哪种暴露途径,所有这6种重金属的HQs都低于安全值1,这说明虽然印刷电路板在生产制造过程中会向周边的环境释放一定量的重金属,但是并没有造成明显的非致癌性风险；但是就致癌性风险来说,Cr的致癌性风险值都大于10-6,在3.70×10-5-1.60×10-3之间；而Ni和Cd的致癌性风险值都低于10-6,这表明印刷电路板的生产车间中Cr会对生产工人造成致癌风险。这对印刷电路板生产原料、生产工艺和现场保护措施提出了新的挑战。
采集印刷电路板企业周边环境土壤和灰尘样品,分析发现土壤样品中∑11PBDE(不包含BDE-209)污染浓度范围为1.00～18.43ng/g dw(平均值7.23ng/g dw)；BDE-209污染浓度范围为3.50～330.0ng/g dw(平均值69.88ng/g dw)。林地土壤中PBDEs同系物分布主要以BDE-209为最主要污染物,其含量占77.82%～96.45%,平均为86.57%。灰尘中∑11PBDE(不包含BDE-209)污染浓度范围为16.00～258.2ng/g dw(平均值113.8ng/gdw); BDE-209污染浓度范围为216.1～1947ng/g dw(平均值983.8ng/g dw)。灰尘中PBDEs同系物分布主要以BDE-209为最主要污染物,其含量占67.52%～86.54%,平均为76.57%。电路板厂向四个方向的扩散基本呈现出PBDEs浓度随距离增大而逐渐降低的趋势。这说明PBDEs的释放源与电路板厂生产有关,但总的来说影响较小。此外,采样点周边环境如建筑工地出现了PBDEs浓度的跳跃现象,表明PBDEs释放源的多样性。
在污水处理厂所有污泥样品中都有PBDEs检出：各构筑物污泥中PBDEs浓度范围都在4226.76-9204.14ng/g dw之间。其中,BDE-209是主导同系物,在所有PBDEs浓度之和所占的平均比例为83.16%,其比例范围为75.75-89.48%。接下来分别是：BDE-99>BDE-47>BDE-28,BDE-183,和BDE-153>BDE-15,BDE-100,BDE-154和BDE-206>BDE-203,BDE-207和BDE-208。该污水处理厂的进水样品中溶解态PBDEs总浓度为183.11ng/L,而改污水处理厂的最终出水样品中溶解态PBDEs浓度则降至7.07ng/L, PBDEs的去除率达到96%以上。所有污水样品中BDE-209都是最主要的同系物,所占浓度比例在75.75%-85.68%之间,BDE-99和BDE-47是仅次于BDE-209的另外2种主要同系物。通过对污水处理流程中PBDEs的溶解态和颗粒态分配系数的研究得出,溶解性颗粒物对疏水性有机物在整个污水处理流程中的迁移、转化有重要的影响。该污水厂的日均PBDEs负荷量为21311.2mg/d,污水经初沉池和二沉池处理之后分别有58.07%和39.91%的PBDEs被去除,即一共有97.98%的PBDEs被去除了,最后在出水中只剩2.02%的PBDEs。该污水厂通过出水的日均排放PBDEs的量为430.8mg,通过脱水污泥日均排放PBDEs的量高达20880.4mg。土壤在污泥农用之后PBDEs浓度年增加量为25.4ng/g,污泥农用需要百年以上才能达到欧盟的规定限值。污水厂出水接纳河流表层沉积物中检测到了较高的PBDEs,而且在距离出水口下游5km处仍然能检测出比上游0.2km处高的PBDEs,说明污水处理厂出水对接纳河流水体沉积物中PBDEs影响显著,是其PBDEs的一个主要污染源。
在所采集的太湖28个采样点的样品中,检出率最高的是BDE-209、-47和-99,平均浓度分别为22.72、0.124和0.279ng/g dw。其中,BDE-209的浓度最高,占总浓度的80%以上；除去BDE-209之外,占∑7PBDEs总浓度比例最高的两个是BDE-47和-99,分别占44.65%和24.24%。PBDEs浓度与样品的TOC值之间的相关性较差,表明太湖沉积物中的PBDEs分布不仅受沉积物中TOC影响,而且还受其他迁移、转化的机制影响。沉积物中PBDEs同系物组成显示其主要来源于商业十溴和商业五溴产品。太湖沉积物中PBDEs的浓度在近10年增长迅速,且没有放缓的趋势。太湖沉积物中∑25PBDEs和BDE-209的赋存量估值分别为3668.48kg和26296.61kg。太湖表层沉积物中Cu的浓度在20.79-113.79mg/kg之间,平均浓度为62.04±30.43mg/kg；Zn的浓度在80.7-285.10mg/kg之间,平均浓度为144.92±45.57mg/kg；Pb的浓度在57.28-117.52mg/kg之间,平均浓度为88.84±15.04mg/kg；Cd的浓度在0.09-1.00mg/kg之间,平均浓度为0.53±0.26mg/kg；Ni的浓度在33.45-82.54mg/kg之间,平均浓度为56.84±15.16mg/kg。相关性分析表明,太湖表层沉积物中重金属除了r(Cu,Zn)=0.46和r(Cd,Pb)=-0.382之外,其他重金属之间的相关性都不明显。这说明太湖沉积物中哥重金属元素的的来源非常不一致；而且受到人为活动影响极大,人为活动所排放的重金属已经远远高于其背景值。另外,主成分分析表明太湖表层沉积物主要受人类生活生产污水、大气沉降和矿石自然风化侵蚀这三个因素的影响。
东海表层沉积物中∑PBDEs的浓度范围为0.20-2.09ng/g dw,BDE-209的浓度范围为0.57-2.87ng/g dw。东海表层沉积物中BDE-209在所有PBDEs中所占浓度百分比范围为57.9-76.7%,接下来分别是BDE-99和BDE-47,所占比例范围分别为11.7-21.5%和7.1-17.4%。PBDEs主要来源于内陆河流的输送和大气沉降,其分布受海流方向、TOC和大气沉降共同影响。其分布呈现出(离海岸线)由近及远浓度越来越低的趋势；由北到南浓度上升的趋势。东海柱状沉积物中PBDEs浓度很好的反应出了PBDEs在中国大陆的使用历史和现状,其浓度呈现出先上升后下降的趋势,说明相关法令对PBDEs的使用具有决定性影响。表层沉积物TOC含量在0.54-0.88%之间,柱状沉积物TOC的含量在0.62-0.88%之间,而且不管是表层沉积物(R2=0.723,p<0.01)还是柱状沉积物(R2=0.595,p<0.01),PBDEs浓度和TOC含量之间有较强的线性关系都非常好,这进一步验证了东海沉积物中PBDEs浓度分布的一个重要影响因素就是沉积物中TOC含量。
PCB (Printed Circuit Boards) industry are the most active industry among the Contemporary Electronic Components Industry. According to investigation of the China Electronics industry Association, the PCB production output value of China in2003was￥50.069billion, which is more than the United States, after Japan, ranking second in the world. On the other hand, due to the severe pollution of PCB industry, a large number of PCB manufactory were moved into China from other country, such as Japan, South Korea and so on, which make the Heavy metals and PBDEs pollution more aggravated in China. However, there were few study focus on the pollution which was made during the PCB process. So, our study is made to focus on the Heavy metals and PBDEs pollution during the PCB process.
In this study, reliable analysis and instrument method for qualitative and quantitative determination of Heavy metals and PBDEs in different environment mediums were built up. After literature survey and field investigation, we chose a typical PCB manufacturing enterprises as our main research object. Then we sampling raw material, wastewater, sludge, particular matters and dust during the PCB process. In raw material, Cu is the highest concentration metal, which concentration is between28000-438000mg/kg, followed by Zn> Pb> Ni> Cd. There is almost none of PBDEs. In wastewater, Cu (1.14±0.71mg/L) is the highest concentration metal, followed by Pb (0.09±0.03mg/L), Ni (0.04±0.01mg/L) and Cd (N.D.). There is almost none of PBDEs. In sludge, Cu ((1.71±0.49)×105mg/kg dw) is the highest concentration metal, followed by Ni (1640.36±484.77mg/kg dw), Pb (791.63±112.05mg/kg dw) and Cd (N.D.). The concentration of PBDEs in wastewater is0.02±0.01mg/kg dw, respectively.
The concentration of TSP (total suspended particulate matter), PM10and PM2.5(particular matter diameter below10and2.5μm) in the workshop atmosphere during the PCB process are6.1-365.3,27.1-289.8and22.1-212.3μg/m3, respectively. The correlation between TSP, PM10and PM2.5is very well, and the proportion of PM2.5in TSP is between50%and80%.In TSP, PM10and PM2.5, Zn is the highest concentration metal, followed by Cu>Pb≈Cr> Ni> Cd. There is almost none of PBDEs in PM10.
The particle size range of dust in the workshop during the PCB process is between0.3and750μm, in which the proportion of PM2.5and PM10are5.59-10.72%and14.22-26.15%, respectively. The volume average diameter (D(4,3)) of dust sample are in the following order: Drilling (47.83μm)> Raw materials warehouse (44.11μm)> Lamination (41.53μm)> Profiling (37.37μm)> Milling (32.76μm)> Cut lamination (31.23μm). In dust, Cu (6.54-56.31mg/g) is the highest concentration metal, followed by Zn (0.77-4.47mg/g), Pb (0.26-0.49mg/g), Cr (0.39-1.59mg/g), Ni (0.13-0.41mg/g) and Cd (nd-0.056mg/g). There is almost none of PBDEs in dust except a little of BDE-209. Then we take a risk assessment about the six heavy metal in each workshop, the HQ value for each non-carcinogenic metal via all three exposed way (ingestion, inhalation and dermal contact) are all below the safe value1, it indicated that there are no obvious non-carcinogenic risk for each heavy metal. However, the carcinogenic risk for Cr are between3.70×l0-5and1.60×10-3,which is higher than the safe value10-6, the carcinogenic risk for Ni and Cd are all below the safe value10-6, it indicated that there are some carcinogenic risk for Cr.
In soil samples collect around the PCB manufactory, the concentration of∑11PBDE (except BDE-209) are among1.00to18.43ng/g dw, average concentration is7.23ng/g dw; The concentration of BDE-209are among3.50to330.0ng/g dw, average concentration is69.88ng/g dw. Obviously, BDE-209is the major congeners, and it contribution77.82%～96.45%(average:86.57%) for the total PBDEs. In dust samples collect around the PCB manufactory, the concentration of∑11PBDE (except BDE-209) are among16.00to258.2ng/g dw, average concentration is113.8ng/g dw; The concentration of BDE-209are among216.1to1947ng/g dw, average concentration is983.8ng/g dw. Similar to PBDEs in soil sample, BDE-209is also the major congeners, and it contribution67.52%～86.54%(average:76.57%) for the total PBDEs. PBDEs concentration decreases gradually with the increase of distance, the sampling site far from the PCB manufactory. This indicate that the PCB manufactory is the source of PBDEs release. Moreover, there are some abrupt phenomenon within PBDEs in soil samples, this indicate that PCB manufactory is not the only source of PBDEs release, there are some other source.
In sludge samples collected from a typical Sewage Treatment Plant, PBDEs concentration are between4226.76and9204.14ng/g dw. BDE-209is the dominate congeners, which contribute75.75～89.48%of the total PBDEs, followed by BDE-99> BDE-47> BDE-28, BDE-183, and BDE-153> BDE-15, BDE-100, BDE-154and BDE-206> BDE-203, BDE-207and BDE-208. PBDEs concentration in influent and effluent are183.11ng/L and7.07ng/L, respectively, indicate about98%of PBDEs in influent is removed during the STP. Similar to PBDEs in sludge, BDE-209is the dominate congeners, which contribute75.75%-85.68%of the total PBDEs, followed by BDE-99and BDE-47. Research about the partition coefficient of PBDEs in solid phase and dissolved phase has shown that soluble particulate matter is a key factor for the migration and transformation of PBDEs during STP process. The mass loading of PBDEs in this STP is estimated as21311.2mg/d. There are58.07%and39.91%of total PBDEs removed from the wastewater when wastewater is treated by primary sedimentation tank and secondary sedimentation tank, in other words, there are only2.02%of PBDEs in effluent. And the mass of PBDEs release via effluent and dewater sludge are estimated as420.8mg/d and20880.4mg/d, respectively. The PBDEs in sediment from the Wastewater Receiving Stream indicate that effluent of STP is a source of PBDEs release.
Twenty-eight sediment samples were collected from the Taihu Lake and analyzed to acquire information about the levels, distribution, possible sources, time trend and inventory of polybrominated diphenyl ethers (PBDEs) in the Taihu Lake. Our results showed that the most abundant BDE congeners in surface sediments were BDE-47,-99and-209, with a median value of0.124,0.279, and22.72ng/g dw, respectively. The levels of BDE-209in our samples were much higher relative to those of the other BDE congeners and made up more than80%of the PBDEs levels in almost all samples. Disregarding BDE209, among the seven PBDEs (BDE-28,-47,-99,-100,-153,-154,-183) more concerned, the most abundant ones were BDE-47and-99, which contributed44.65%(ranged from29.02%to73.11%),24.24%(ranged from2.27%to39.66%) to∑7PBDEs, respectively. The correlation between PBDE and TOC was poor, indicating that PBDEs concentrations in sediments of the Taihu Lake were controlled not only by TOC contents, but also by a combined effect of transport, mixing, depositional mechanisms associated with PBDEs, uncontaminated sediments, or fresh input of PBDEs. As expected, the time trend of PBDEs concentration in surface sediment from Taihu Lake were increasing, and the inventory of E25PBDEs and BDE-209were estimated to be3668kg and26296kg. In the surface sediment from Taihu Lake, the concentration of Cu, Zn, Pb, Cd and Ni are0.79-113.79mg/kg (62.04±30.43mg/kg),80.7-285.10mg/kg (144.92±45.57mg/kg),57.28-117.52mg/kg (88.84±15.04mg/kg),0.09-1.00mg/kg (0.53±0.26mg/kg) and33.45-82.54mg/kg (56.84±15.16mg/kg), respectively. According to the correlation analysis, the correlation among these heavy metals are not well, this indicate that the source of these heavy metals are different. Moreover, the PCA (Principal component analysis) manifest that there are three main source of these heavy metals:Anthropogenic emissions, Atmospheric deposition and Natural weathering.
The concentration of∑PBDEs and BDE-209in surface sediment from East China Sea(ECS) are between0.20to2.09and0.57to2.87ng/g dw, respectively. BDE-209is the dominate congeners, contribute57.9-76.7%of total PBDEs, followed by BDE-99and BDE-47, which contribute11.7-21.5%and7.1-17.4%of total PBDEs, respectively. Moreover, the concentration of PBDEs decreased within the increase of distance between sampling site and coastline, rise from north to south. This indicate that, in surface sediment from ECS, PBDEs are mainly derived from the inland river transportation and atmospheric deposition, and the distribution of PBDEs are influenced by ocean current, TOC (Total Organic Carbon,%) and atmospheric deposition. The concentration of PBDEs in core sediment from ECS is well matching the history and status of PBDEs in China. The TOC content in surface and core sediment from ECS are between0.54to0.88%and0.62to0.88%, respectively. And the correlation between TOC and PBDEs in both surface and core sediment are very well, the correlation coefficient are R2=0.723(p<0.01) and R2=0.595(p<0.01) for surface and core sediment, respectively. This further indicate that TOC is a key factor for the distribution of PBDEs in sediment.
在实验室建立可靠的环境介质中PBDEs和重金属分析检测方法的基础上,通过前期的文献调研、印刷电路板生产企业联系和实地考察,选择了具有代表性的印刷电路板生产企业为我们的主要研究对象。然后,系统采集印刷电路板各生产流程、车间的原料、清洗水、灰尘和大气样品。通过分析得出印刷电路板生产原料中含有不同浓度的重金属,其中Cu的含量最高,在28000-438000mg/kg之间,其他重金属的浓度比Cu低几个数量级,浓度由高低分别是Zn>Pb>Ni>Cd；原料中几乎没有PBDEs。而在其生产过程中产生的污水和污泥中,也检测到了不同浓度的重金属和PBDEs。出水样品中检测出的含量最高的重金属是Cu(1.14±0.71mg/L),接着是Pb(0.09±0.03mg/L),Ni(0.04±0.01mg/L)和Cd(N.D.),而几乎不含有PBDEs;污泥中重金属浓度最高的是Cu,浓度为(1.71±0.49)×105(mg/kg dw),接下来分别是Ni(1640.36±484.77mg/kg dw)、Pb(791.63±112.05mg/kg dw)和Cd(ND),PBDEs浓度为0.02±0.01ng/kg dw。印刷电路板在生产过程中会产生大量的悬浮颗粒物,各车间空气中TSP、PM1o和PM2.5浓度分别在6.1-365.3、27.1-289.8和22.1-212.3μg/m3之间；各车间大气中PM1o和TSP以及PM2.5和PM1o之间的相关性都非常好,而且PM2.5所占比例在50%-80%之间；说明车间大气颗粒物来源一致,另外车间除尘装置对车间空气中颗粒物有很好的去除效果。各车间大气TSP、PM1o和PM2.5中Zn的浓度是最高的,其他金属浓度由高到低依次是Cu>Pb≈Cr>Ni>Cd。
印刷电路企业各车间灰尘样品的粒径范围在0.3-750μm之间。其中PM2.5和PM1o所占百分比分别在5.59-10.72%和14.22-26.15%之间。各个车间灰尘样品的体积平均直径D(4,3)从大到小依次为：钻孔车间(47.83gm)>原料仓库(44.11μm)>压合车间(41.53μm)>成型车间(37.371μm)>捞边车间(32.76μm)>下料车间(31.23μm)。灰尘中浓度最高的重金属是Cu,其浓度范围为6.54-56.31mg/g；其他金属浓度由高到低依次是Zn、Pb、Cr、Ni和Cd,其浓度范围分别为0.77-4.47,0.26-0.49,0.39-1.59,0.13-0.41和nd-0.056mg/g。各采样点的灰尘中均没有检出低溴代的BDEs,而只检测出少量的BDE-209。而就TBBPA来说,各车间的浓度差异较大,浓度在125-9091ng/g之间。另外,类似于RoHHS指令一样的相关法令对部分重金属(Pb)和溴系阻燃剂在印刷电路板生产工艺中的使用有决定性的影响。通过灰尘和空气颗粒物中重金属的浓度和相关风险评价模型对各车间进行风险评价发现：就各重金属的非致癌性风险来说,不管是哪种暴露途径,所有这6种重金属的HQs都低于安全值1,这说明虽然印刷电路板在生产制造过程中会向周边的环境释放一定量的重金属,但是并没有造成明显的非致癌性风险；但是就致癌性风险来说,Cr的致癌性风险值都大于10-6,在3.70×10-5-1.60×10-3之间；而Ni和Cd的致癌性风险值都低于10-6,这表明印刷电路板的生产车间中Cr会对生产工人造成致癌风险。这对印刷电路板生产原料、生产工艺和现场保护措施提出了新的挑战。
采集印刷电路板企业周边环境土壤和灰尘样品,分析发现土壤样品中∑11PBDE(不包含BDE-209)污染浓度范围为1.00～18.43ng/g dw(平均值7.23ng/g dw)；BDE-209污染浓度范围为3.50～330.0ng/g dw(平均值69.88ng/g dw)。林地土壤中PBDEs同系物分布主要以BDE-209为最主要污染物,其含量占77.82%～96.45%,平均为86.57%。灰尘中∑11PBDE(不包含BDE-209)污染浓度范围为16.00～258.2ng/g dw(平均值113.8ng/gdw); BDE-209污染浓度范围为216.1～1947ng/g dw(平均值983.8ng/g dw)。灰尘中PBDEs同系物分布主要以BDE-209为最主要污染物,其含量占67.52%～86.54%,平均为76.57%。电路板厂向四个方向的扩散基本呈现出PBDEs浓度随距离增大而逐渐降低的趋势。这说明PBDEs的释放源与电路板厂生产有关,但总的来说影响较小。此外,采样点周边环境如建筑工地出现了PBDEs浓度的跳跃现象,表明PBDEs释放源的多样性。
在污水处理厂所有污泥样品中都有PBDEs检出：各构筑物污泥中PBDEs浓度范围都在4226.76-9204.14ng/g dw之间。其中,BDE-209是主导同系物,在所有PBDEs浓度之和所占的平均比例为83.16%,其比例范围为75.75-89.48%。接下来分别是：BDE-99>BDE-47>BDE-28,BDE-183,和BDE-153>BDE-15,BDE-100,BDE-154和BDE-206>BDE-203,BDE-207和BDE-208。该污水处理厂的进水样品中溶解态PBDEs总浓度为183.11ng/L,而改污水处理厂的最终出水样品中溶解态PBDEs浓度则降至7.07ng/L, PBDEs的去除率达到96%以上。所有污水样品中BDE-209都是最主要的同系物,所占浓度比例在75.75%-85.68%之间,BDE-99和BDE-47是仅次于BDE-209的另外2种主要同系物。通过对污水处理流程中PBDEs的溶解态和颗粒态分配系数的研究得出,溶解性颗粒物对疏水性有机物在整个污水处理流程中的迁移、转化有重要的影响。该污水厂的日均PBDEs负荷量为21311.2mg/d,污水经初沉池和二沉池处理之后分别有58.07%和39.91%的PBDEs被去除,即一共有97.98%的PBDEs被去除了,最后在出水中只剩2.02%的PBDEs。该污水厂通过出水的日均排放PBDEs的量为430.8mg,通过脱水污泥日均排放PBDEs的量高达20880.4mg。土壤在污泥农用之后PBDEs浓度年增加量为25.4ng/g,污泥农用需要百年以上才能达到欧盟的规定限值。污水厂出水接纳河流表层沉积物中检测到了较高的PBDEs,而且在距离出水口下游5km处仍然能检测出比上游0.2km处高的PBDEs,说明污水处理厂出水对接纳河流水体沉积物中PBDEs影响显著,是其PBDEs的一个主要污染源。
在所采集的太湖28个采样点的样品中,检出率最高的是BDE-209、-47和-99,平均浓度分别为22.72、0.124和0.279ng/g dw。其中,BDE-209的浓度最高,占总浓度的80%以上；除去BDE-209之外,占∑7PBDEs总浓度比例最高的两个是BDE-47和-99,分别占44.65%和24.24%。PBDEs浓度与样品的TOC值之间的相关性较差,表明太湖沉积物中的PBDEs分布不仅受沉积物中TOC影响,而且还受其他迁移、转化的机制影响。沉积物中PBDEs同系物组成显示其主要来源于商业十溴和商业五溴产品。太湖沉积物中PBDEs的浓度在近10年增长迅速,且没有放缓的趋势。太湖沉积物中∑25PBDEs和BDE-209的赋存量估值分别为3668.48kg和26296.61kg。太湖表层沉积物中Cu的浓度在20.79-113.79mg/kg之间,平均浓度为62.04±30.43mg/kg；Zn的浓度在80.7-285.10mg/kg之间,平均浓度为144.92±45.57mg/kg；Pb的浓度在57.28-117.52mg/kg之间,平均浓度为88.84±15.04mg/kg；Cd的浓度在0.09-1.00mg/kg之间,平均浓度为0.53±0.26mg/kg；Ni的浓度在33.45-82.54mg/kg之间,平均浓度为56.84±15.16mg/kg。相关性分析表明,太湖表层沉积物中重金属除了r(Cu,Zn)=0.46和r(Cd,Pb)=-0.382之外,其他重金属之间的相关性都不明显。这说明太湖沉积物中哥重金属元素的的来源非常不一致；而且受到人为活动影响极大,人为活动所排放的重金属已经远远高于其背景值。另外,主成分分析表明太湖表层沉积物主要受人类生活生产污水、大气沉降和矿石自然风化侵蚀这三个因素的影响。
东海表层沉积物中∑PBDEs的浓度范围为0.20-2.09ng/g dw,BDE-209的浓度范围为0.57-2.87ng/g dw。东海表层沉积物中BDE-209在所有PBDEs中所占浓度百分比范围为57.9-76.7%,接下来分别是BDE-99和BDE-47,所占比例范围分别为11.7-21.5%和7.1-17.4%。PBDEs主要来源于内陆河流的输送和大气沉降,其分布受海流方向、TOC和大气沉降共同影响。其分布呈现出(离海岸线)由近及远浓度越来越低的趋势；由北到南浓度上升的趋势。东海柱状沉积物中PBDEs浓度很好的反应出了PBDEs在中国大陆的使用历史和现状,其浓度呈现出先上升后下降的趋势,说明相关法令对PBDEs的使用具有决定性影响。表层沉积物TOC含量在0.54-0.88%之间,柱状沉积物TOC的含量在0.62-0.88%之间,而且不管是表层沉积物(R2=0.723,p<0.01)还是柱状沉积物(R2=0.595,p<0.01),PBDEs浓度和TOC含量之间有较强的线性关系都非常好,这进一步验证了东海沉积物中PBDEs浓度分布的一个重要影响因素就是沉积物中TOC含量。
PCB (Printed Circuit Boards) industry are the most active industry among the Contemporary Electronic Components Industry. According to investigation of the China Electronics industry Association, the PCB production output value of China in2003was￥50.069billion, which is more than the United States, after Japan, ranking second in the world. On the other hand, due to the severe pollution of PCB industry, a large number of PCB manufactory were moved into China from other country, such as Japan, South Korea and so on, which make the Heavy metals and PBDEs pollution more aggravated in China. However, there were few study focus on the pollution which was made during the PCB process. So, our study is made to focus on the Heavy metals and PBDEs pollution during the PCB process.
In this study, reliable analysis and instrument method for qualitative and quantitative determination of Heavy metals and PBDEs in different environment mediums were built up. After literature survey and field investigation, we chose a typical PCB manufacturing enterprises as our main research object. Then we sampling raw material, wastewater, sludge, particular matters and dust during the PCB process. In raw material, Cu is the highest concentration metal, which concentration is between28000-438000mg/kg, followed by Zn> Pb> Ni> Cd. There is almost none of PBDEs. In wastewater, Cu (1.14±0.71mg/L) is the highest concentration metal, followed by Pb (0.09±0.03mg/L), Ni (0.04±0.01mg/L) and Cd (N.D.). There is almost none of PBDEs. In sludge, Cu ((1.71±0.49)×105mg/kg dw) is the highest concentration metal, followed by Ni (1640.36±484.77mg/kg dw), Pb (791.63±112.05mg/kg dw) and Cd (N.D.). The concentration of PBDEs in wastewater is0.02±0.01mg/kg dw, respectively.
The concentration of TSP (total suspended particulate matter), PM10and PM2.5(particular matter diameter below10and2.5μm) in the workshop atmosphere during the PCB process are6.1-365.3,27.1-289.8and22.1-212.3μg/m3, respectively. The correlation between TSP, PM10and PM2.5is very well, and the proportion of PM2.5in TSP is between50%and80%.In TSP, PM10and PM2.5, Zn is the highest concentration metal, followed by Cu>Pb≈Cr> Ni> Cd. There is almost none of PBDEs in PM10.
The particle size range of dust in the workshop during the PCB process is between0.3and750μm, in which the proportion of PM2.5and PM10are5.59-10.72%and14.22-26.15%, respectively. The volume average diameter (D(4,3)) of dust sample are in the following order: Drilling (47.83μm)> Raw materials warehouse (44.11μm)> Lamination (41.53μm)> Profiling (37.37μm)> Milling (32.76μm)> Cut lamination (31.23μm). In dust, Cu (6.54-56.31mg/g) is the highest concentration metal, followed by Zn (0.77-4.47mg/g), Pb (0.26-0.49mg/g), Cr (0.39-1.59mg/g), Ni (0.13-0.41mg/g) and Cd (nd-0.056mg/g). There is almost none of PBDEs in dust except a little of BDE-209. Then we take a risk assessment about the six heavy metal in each workshop, the HQ value for each non-carcinogenic metal via all three exposed way (ingestion, inhalation and dermal contact) are all below the safe value1, it indicated that there are no obvious non-carcinogenic risk for each heavy metal. However, the carcinogenic risk for Cr are between3.70×l0-5and1.60×10-3,which is higher than the safe value10-6, the carcinogenic risk for Ni and Cd are all below the safe value10-6, it indicated that there are some carcinogenic risk for Cr.
In soil samples collect around the PCB manufactory, the concentration of∑11PBDE (except BDE-209) are among1.00to18.43ng/g dw, average concentration is7.23ng/g dw; The concentration of BDE-209are among3.50to330.0ng/g dw, average concentration is69.88ng/g dw. Obviously, BDE-209is the major congeners, and it contribution77.82%～96.45%(average:86.57%) for the total PBDEs. In dust samples collect around the PCB manufactory, the concentration of∑11PBDE (except BDE-209) are among16.00to258.2ng/g dw, average concentration is113.8ng/g dw; The concentration of BDE-209are among216.1to1947ng/g dw, average concentration is983.8ng/g dw. Similar to PBDEs in soil sample, BDE-209is also the major congeners, and it contribution67.52%～86.54%(average:76.57%) for the total PBDEs. PBDEs concentration decreases gradually with the increase of distance, the sampling site far from the PCB manufactory. This indicate that the PCB manufactory is the source of PBDEs release. Moreover, there are some abrupt phenomenon within PBDEs in soil samples, this indicate that PCB manufactory is not the only source of PBDEs release, there are some other source.
In sludge samples collected from a typical Sewage Treatment Plant, PBDEs concentration are between4226.76and9204.14ng/g dw. BDE-209is the dominate congeners, which contribute75.75～89.48%of the total PBDEs, followed by BDE-99> BDE-47> BDE-28, BDE-183, and BDE-153> BDE-15, BDE-100, BDE-154and BDE-206> BDE-203, BDE-207and BDE-208. PBDEs concentration in influent and effluent are183.11ng/L and7.07ng/L, respectively, indicate about98%of PBDEs in influent is removed during the STP. Similar to PBDEs in sludge, BDE-209is the dominate congeners, which contribute75.75%-85.68%of the total PBDEs, followed by BDE-99and BDE-47. Research about the partition coefficient of PBDEs in solid phase and dissolved phase has shown that soluble particulate matter is a key factor for the migration and transformation of PBDEs during STP process. The mass loading of PBDEs in this STP is estimated as21311.2mg/d. There are58.07%and39.91%of total PBDEs removed from the wastewater when wastewater is treated by primary sedimentation tank and secondary sedimentation tank, in other words, there are only2.02%of PBDEs in effluent. And the mass of PBDEs release via effluent and dewater sludge are estimated as420.8mg/d and20880.4mg/d, respectively. The PBDEs in sediment from the Wastewater Receiving Stream indicate that effluent of STP is a source of PBDEs release.
Twenty-eight sediment samples were collected from the Taihu Lake and analyzed to acquire information about the levels, distribution, possible sources, time trend and inventory of polybrominated diphenyl ethers (PBDEs) in the Taihu Lake. Our results showed that the most abundant BDE congeners in surface sediments were BDE-47,-99and-209, with a median value of0.124,0.279, and22.72ng/g dw, respectively. The levels of BDE-209in our samples were much higher relative to those of the other BDE congeners and made up more than80%of the PBDEs levels in almost all samples. Disregarding BDE209, among the seven PBDEs (BDE-28,-47,-99,-100,-153,-154,-183) more concerned, the most abundant ones were BDE-47and-99, which contributed44.65%(ranged from29.02%to73.11%),24.24%(ranged from2.27%to39.66%) to∑7PBDEs, respectively. The correlation between PBDE and TOC was poor, indicating that PBDEs concentrations in sediments of the Taihu Lake were controlled not only by TOC contents, but also by a combined effect of transport, mixing, depositional mechanisms associated with PBDEs, uncontaminated sediments, or fresh input of PBDEs. As expected, the time trend of PBDEs concentration in surface sediment from Taihu Lake were increasing, and the inventory of E25PBDEs and BDE-209were estimated to be3668kg and26296kg. In the surface sediment from Taihu Lake, the concentration of Cu, Zn, Pb, Cd and Ni are0.79-113.79mg/kg (62.04±30.43mg/kg),80.7-285.10mg/kg (144.92±45.57mg/kg),57.28-117.52mg/kg (88.84±15.04mg/kg),0.09-1.00mg/kg (0.53±0.26mg/kg) and33.45-82.54mg/kg (56.84±15.16mg/kg), respectively. According to the correlation analysis, the correlation among these heavy metals are not well, this indicate that the source of these heavy metals are different. Moreover, the PCA (Principal component analysis) manifest that there are three main source of these heavy metals:Anthropogenic emissions, Atmospheric deposition and Natural weathering.
The concentration of∑PBDEs and BDE-209in surface sediment from East China Sea(ECS) are between0.20to2.09and0.57to2.87ng/g dw, respectively. BDE-209is the dominate congeners, contribute57.9-76.7%of total PBDEs, followed by BDE-99and BDE-47, which contribute11.7-21.5%and7.1-17.4%of total PBDEs, respectively. Moreover, the concentration of PBDEs decreased within the increase of distance between sampling site and coastline, rise from north to south. This indicate that, in surface sediment from ECS, PBDEs are mainly derived from the inland river transportation and atmospheric deposition, and the distribution of PBDEs are influenced by ocean current, TOC (Total Organic Carbon,%) and atmospheric deposition. The concentration of PBDEs in core sediment from ECS is well matching the history and status of PBDEs in China. The TOC content in surface and core sediment from ECS are between0.54to0.88%and0.62to0.88%, respectively. And the correlation between TOC and PBDEs in both surface and core sediment are very well, the correlation coefficient are R2=0.723(p<0.01) and R2=0.595(p<0.01) for surface and core sediment, respectively. This further indicate that TOC is a key factor for the distribution of PBDEs in sediment.
引文
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