受体模型应用于典型环境介质中多环芳烃、二噁英和多氯联苯的来源解析研究
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摘要
受体模型是通过对采样点环境样品(受体)的化学和显微分析,确定各污染源贡献率的一系列技术。受体模型的最终目的是识别对受体有贡献的污染源,并且定量计算各污染源的分担率。本研究对非负约束的因子分析模型(FA-NNC)进行了改进,以多环芳烃(PAHs),多氯代二苯并二噁英/呋喃(PCDD/Fs)和多氯联苯(PCBs)这三种典型的持久性有毒物质为研究对象,对气相中的PAHs(大连地区大气)、植物相中的PCDD/Fs和PCBs(大连地区松针)和沉积物相中的PAHs(白洋淀沉积物)的污染水平、组成和分布进行了研究,并使用FA-NNC对它们在各环境介质中的来源进行了深入的分析。
FA-NNC是一种较为先进的受体模型,在实际应用中有研究者发现FA-NNC在非负约束的因子旋转过程中可能会由于不收敛,而最终导致无法进行来源解析,本研究对FA-NNC模型的迭代终止判定条件进行了优化,并采用人工模拟数据对改进后的模型进行了考查,改进后的FA-NNC较好的解析出了预设的4个主要的污染源指纹谱图及其贡献率。通过改进前后FA-NNC应用于实测数据的结果比较,发现改进后的模型能够提供更多的污染源信息,并且更好的复原了污染源的指纹谱图。改进后FA-NNC模型的结果与PMF的结果比较发现,改进后FA-NNC的结果与PMF的结果基本一致,说明改进后FA-NNC可以有效进行污染物的来源解析。
植物相中PCDD/Fs和PCBs的来源解析——以大连地区松针为例。对大连地区松针中PCDD/Fs和PCBs浓度数据分析发现,PCDD/Fs在各个采样点的浓度分布较为均匀,松针中的PCBs主要是以低氯代(三氯取代、四氯取代和五氯取代)的PCBs为主,且大连松针中PCBs的组成与我国PCBs产品的组成较为相似。通过FA-NNC和PMF对松针中PCDD/Fs和PCBs进行解析发现,对于松针中的PCDD/Fs,解析得到了4个主要的污染源,分别为燃烧过程的排放(58%～74%),五氯酚的污染(15%～17%),金属冶炼(9%～12%)和交通尾气排放(2%～13%);对于松针中的PCBs的源解析发现,国产多氯联苯产品PCB3和PCB5的挥发是PCBs的主要来源,它们的贡献率分别约为80%和20%,该结果基本与我国生产的多氯联苯产品PCB3(9000吨)和PCB5(1000吨)的产量比基本一致。
气相中PAHs的监测和来源解析——以大连地区大气为例。通过对大连地区大气中PAHs的采样和监测分析发现,该地区大气中PAHs的污染并不严重,平均浓度低于中国北方的北京,天津,沈阳等城市。并且PAHs的浓度有明显的季节性变化,在采暖期PAHs的浓度较高,而在非采暖期PAHs的浓度较低。本研究使用FA-NNC模型结合大连当地的PAHs污染源指纹谱图和文献报道的指纹谱图的方法,很好的解析了大连大气PM_(10)中PAHs的来源。FA-NNC模型解析的结果表明,在采暖期大连大气PM_(10)中PAHs主要来自燃煤相关污染源(89%),其次是交通排放(11%),而在非采暖期大连大气PM_(10)中PAHs主要来自交通排放(79%),其次是燃煤电厂的排放(21%)。
沉积物相中PAHs的监测和来源解析——以白洋淀沉积物为例。通过对白洋淀地区沉积物中PAHs的野外采样分析表明,白洋淀地区沉积物中PAHs的浓度较低,说明白洋淀地区沉积物受到的PAHs污染相对较轻。上层和下层沉积物中PAHs的组成有较大的差别,上层沉积物样品中含高环的PAHs较多,而下层沉积物中低环PAHs占很大比例,表明白洋淀地区PAHs的主要污染源随着时间的推移也在发生变化。通过FA-NNC对沉积物PAHs的来源解析的表明,白洋淀地区长期以来的主要PAHs污染源是居民燃煤和生物质燃烧,其贡献率分别为31%和39%,其次是近30年新出现的燃煤电厂和交通污染源,它们的贡献率约分别是17%和13%。
Receptor models assess contributions from all the major sources based on observations at sampling sites,the "receptors".Receptor models have been widely used for source apportionment of pollutants in various environmental media.Many different receptor modeling methods are available,such as factor analysis/multiple linear regression(FA/MLR), chemical mass balance(CMB),positive matrix factorization(PMF) and factor analysis with non-negative constraints(FA-NNC).In this study,FA-NNC was modified and verified its applicability.The levels,compositions and sources of atmospheric polycyclic aromatic hydrocarbons(PAHs),pine needle polychlorinated dibenzo-p-dioxins/ dibenzofurans (PCDD/Fs) and polychlorinated biphenyls(PCBs) in Dalian and sediment PAHs in Baiyangdian were investigated.FA-NNC and PMF were adopted to apportion their sources.
FA-NNC is one of the advanced receptor models.It has been used for source apportionment of organic pollutants by many researchers.However,it was reported that in some cases,FA-NNC could not converge,indicating the limits of the robustness of FA-NNC. In this study,FA-NNC was modified and verified by using artificial data set created by Monte Carlo simulation and real world data set.The robustness of FA-NNC was enhanced after modification.Furthermore,the model can offer more information of the pollution source and successfully predict the source fingerprints.Positive matrix factorization(PMF) was used to verify the effectiveness of the modified FA-NNC.Results from PMF and the modified FA-NNC were consistent,indicating the effectiveness of the modified FA-NNC.
It was successful to employ FA-NNC and PMF for source apportionment of PCDD/Fs and PCBs in pine needles in Dalian.The source profiles derived from the two receptor-models were almost the same.In Dalian,the main sources of PCDD/Fs were estimated to be various combustion processes(58%～74%),PCP contamination(15%～17%), metal metallurgy(9%～12%),and traffic emissions(2%～13%).As for PCBs,two similar source profiles were identified by the two receptor-models.One source profile that is similar to Aroclor1242 represents China's technical PCB product PCB3(72%～80%),and another source profile that is similar to Aroclor1254 represents the product PCB5(20%～28%).The source contributions are qualitatively consistent with the proportions of technical PCB products synthesized and used in China.
The average PAH levels in Dalian was comparable to that found in some international cities and lower than those reported for several northern Chinese cities.Obvious seasonal variations in the PAH concentrations were observed,with maximum and minimum concentrations in heating and non-heating period,respectively.It was successful to employ FA-NNC combined with local and literature PAH source profiles for source apportionment of atmospheric PAHs.The source apportionment results by the FA model with nonnegative constraints showed that PAHs originated from coal related sources mainly(89%) and followed by traffic emissions(11%) in heating period,and in non-heating period,traffic emissions is the major PAH contributor(79%),and coal-fired power plant as a second source (21%).
The average sediment PAH level in Baiyangdian area was lower than that found in some other sediment samples worldwide.This indicates that the environment of Baiyangdian area was slightly contaminated by PAHs.Distinct patterns were found in upper and lower sediment samples,with high molecular weight PAHs(5 or 6 rings) mainly in upper sediment samples and low molecular weight PAHs(2 or 3 rings) in lower sediment samples,which indicated that the main sources of PAHs were changing with time.Results of FA-NNC showed that residential coal(31%) and biomass burning(39%) were the main PAH source in Baiyangdian area,followed by coal fired power plants(17%) and traffic emissions(13%).
FA-NNC是一种较为先进的受体模型,在实际应用中有研究者发现FA-NNC在非负约束的因子旋转过程中可能会由于不收敛,而最终导致无法进行来源解析,本研究对FA-NNC模型的迭代终止判定条件进行了优化,并采用人工模拟数据对改进后的模型进行了考查,改进后的FA-NNC较好的解析出了预设的4个主要的污染源指纹谱图及其贡献率。通过改进前后FA-NNC应用于实测数据的结果比较,发现改进后的模型能够提供更多的污染源信息,并且更好的复原了污染源的指纹谱图。改进后FA-NNC模型的结果与PMF的结果比较发现,改进后FA-NNC的结果与PMF的结果基本一致,说明改进后FA-NNC可以有效进行污染物的来源解析。
植物相中PCDD/Fs和PCBs的来源解析——以大连地区松针为例。对大连地区松针中PCDD/Fs和PCBs浓度数据分析发现,PCDD/Fs在各个采样点的浓度分布较为均匀,松针中的PCBs主要是以低氯代(三氯取代、四氯取代和五氯取代)的PCBs为主,且大连松针中PCBs的组成与我国PCBs产品的组成较为相似。通过FA-NNC和PMF对松针中PCDD/Fs和PCBs进行解析发现,对于松针中的PCDD/Fs,解析得到了4个主要的污染源,分别为燃烧过程的排放(58%～74%),五氯酚的污染(15%～17%),金属冶炼(9%～12%)和交通尾气排放(2%～13%);对于松针中的PCBs的源解析发现,国产多氯联苯产品PCB3和PCB5的挥发是PCBs的主要来源,它们的贡献率分别约为80%和20%,该结果基本与我国生产的多氯联苯产品PCB3(9000吨)和PCB5(1000吨)的产量比基本一致。
气相中PAHs的监测和来源解析——以大连地区大气为例。通过对大连地区大气中PAHs的采样和监测分析发现,该地区大气中PAHs的污染并不严重,平均浓度低于中国北方的北京,天津,沈阳等城市。并且PAHs的浓度有明显的季节性变化,在采暖期PAHs的浓度较高,而在非采暖期PAHs的浓度较低。本研究使用FA-NNC模型结合大连当地的PAHs污染源指纹谱图和文献报道的指纹谱图的方法,很好的解析了大连大气PM_(10)中PAHs的来源。FA-NNC模型解析的结果表明,在采暖期大连大气PM_(10)中PAHs主要来自燃煤相关污染源(89%),其次是交通排放(11%),而在非采暖期大连大气PM_(10)中PAHs主要来自交通排放(79%),其次是燃煤电厂的排放(21%)。
沉积物相中PAHs的监测和来源解析——以白洋淀沉积物为例。通过对白洋淀地区沉积物中PAHs的野外采样分析表明,白洋淀地区沉积物中PAHs的浓度较低,说明白洋淀地区沉积物受到的PAHs污染相对较轻。上层和下层沉积物中PAHs的组成有较大的差别,上层沉积物样品中含高环的PAHs较多,而下层沉积物中低环PAHs占很大比例,表明白洋淀地区PAHs的主要污染源随着时间的推移也在发生变化。通过FA-NNC对沉积物PAHs的来源解析的表明,白洋淀地区长期以来的主要PAHs污染源是居民燃煤和生物质燃烧,其贡献率分别为31%和39%,其次是近30年新出现的燃煤电厂和交通污染源,它们的贡献率约分别是17%和13%。
Receptor models assess contributions from all the major sources based on observations at sampling sites,the "receptors".Receptor models have been widely used for source apportionment of pollutants in various environmental media.Many different receptor modeling methods are available,such as factor analysis/multiple linear regression(FA/MLR), chemical mass balance(CMB),positive matrix factorization(PMF) and factor analysis with non-negative constraints(FA-NNC).In this study,FA-NNC was modified and verified its applicability.The levels,compositions and sources of atmospheric polycyclic aromatic hydrocarbons(PAHs),pine needle polychlorinated dibenzo-p-dioxins/ dibenzofurans (PCDD/Fs) and polychlorinated biphenyls(PCBs) in Dalian and sediment PAHs in Baiyangdian were investigated.FA-NNC and PMF were adopted to apportion their sources.
FA-NNC is one of the advanced receptor models.It has been used for source apportionment of organic pollutants by many researchers.However,it was reported that in some cases,FA-NNC could not converge,indicating the limits of the robustness of FA-NNC. In this study,FA-NNC was modified and verified by using artificial data set created by Monte Carlo simulation and real world data set.The robustness of FA-NNC was enhanced after modification.Furthermore,the model can offer more information of the pollution source and successfully predict the source fingerprints.Positive matrix factorization(PMF) was used to verify the effectiveness of the modified FA-NNC.Results from PMF and the modified FA-NNC were consistent,indicating the effectiveness of the modified FA-NNC.
It was successful to employ FA-NNC and PMF for source apportionment of PCDD/Fs and PCBs in pine needles in Dalian.The source profiles derived from the two receptor-models were almost the same.In Dalian,the main sources of PCDD/Fs were estimated to be various combustion processes(58%～74%),PCP contamination(15%～17%), metal metallurgy(9%～12%),and traffic emissions(2%～13%).As for PCBs,two similar source profiles were identified by the two receptor-models.One source profile that is similar to Aroclor1242 represents China's technical PCB product PCB3(72%～80%),and another source profile that is similar to Aroclor1254 represents the product PCB5(20%～28%).The source contributions are qualitatively consistent with the proportions of technical PCB products synthesized and used in China.
The average PAH levels in Dalian was comparable to that found in some international cities and lower than those reported for several northern Chinese cities.Obvious seasonal variations in the PAH concentrations were observed,with maximum and minimum concentrations in heating and non-heating period,respectively.It was successful to employ FA-NNC combined with local and literature PAH source profiles for source apportionment of atmospheric PAHs.The source apportionment results by the FA model with nonnegative constraints showed that PAHs originated from coal related sources mainly(89%) and followed by traffic emissions(11%) in heating period,and in non-heating period,traffic emissions is the major PAH contributor(79%),and coal-fired power plant as a second source (21%).
The average sediment PAH level in Baiyangdian area was lower than that found in some other sediment samples worldwide.This indicates that the environment of Baiyangdian area was slightly contaminated by PAHs.Distinct patterns were found in upper and lower sediment samples,with high molecular weight PAHs(5 or 6 rings) mainly in upper sediment samples and low molecular weight PAHs(2 or 3 rings) in lower sediment samples,which indicated that the main sources of PAHs were changing with time.Results of FA-NNC showed that residential coal(31%) and biomass burning(39%) were the main PAH source in Baiyangdian area,followed by coal fired power plants(17%) and traffic emissions(13%).
引文
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