降低二次有机碳对大气颗粒物源解析影响的研究
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摘要
化学质量平衡(CMB)模型是根据质量平衡原理建立起来的受体模型,广泛应用于大气颗粒物来源解析研究中。在源解析研究中,由于大气颗粒物中的二次有机碳(SOC)不是一次污染源的排放物,而是由挥发性有机物(VOCs)在大气环境中经过光化学氧化反应生成的,因此难以获得SOC源的成分谱,这样造成了纳入CMB模型进行计算的受体中含有SOC组分,而源类中却没有相应的SOC排放源的成分谱,使源与受体的匹配程度降低,导致CMB模型计算结果的不确定性增大,这是一直困扰着CMB模型的可靠性的重要难题。
本论文针对SOC源成分谱难以确定的难题开展研究,提出了采用OC/EC最小比值法来估算受体颗粒物中SOC的浓度,在此基础上,重新构建受体成分谱,使碳组分在受体和源之间更加匹配,建立了修正的CMB模型方程,有效地解决了二次污染物SOC对CMB模型的影响,也为解决二次颗粒物的源解析提供了可借鉴的技术方法。
针对SOC定量困难及目前缺乏碳分析方法的统一标准(尤其是OC、EC的界定)等问题,本研究对同一样品中的碳组分同步采用元素分析(EA)法和热-光碳反射(TOR)法进行测定,结合两类分析方法的原理,对测量结果进行了比较研究,对因分析方法不同造成的SOC定量的不确定性进行了讨论。提出了有可能可以利用TOR法加热过程中得到的OP含量值校正EA法测得的OC浓度的思想。
利用本论文所建立的方法,对开封、无锡和攀枝花三城市的颗粒物进行了来源解析,并与传统的CMB模型结果进行了比较,结果表明,本论文所建立的源解析方法的结果优于传统CMB模型的结果。
The chemical mass balance (CMB) model, which is based on the principle of mass conservation, is one of several receptor models that have been applied to source apportionment of ambient particulate matter, and has been widely used. However, the presence of secondary organic carbon (SOC) brought uncertainties to the results of source apportionment. SOC, which is formed through atmospheric oxidation of volatile organic compounds, isn't emitted directly from primary sources. It was very difficult to identify the SOC source profile for CMB model. Therefore, SOC made the matching degree of carbon species between identified sources and receptor decreased, and resulted in the source contributions calculated from CMB model had larger uncertainties. SOC, which influenced the reliability of CMB model, has been a difficult problem for a long time.
In this study, we focused on the problem that SOC source profile was difficult to be obtained, and put forward a new method to solve this problem. The content of this method included:Using "OC/EC minimum ratio" method to estimate SOC concentration, reconstructing new receptor profile based on SOC concentration, and modifiying CMB model. New receptor profile made carbon species in receptor match well with those in identified sources. This method reduced the influence of SOC on CMB model results, and provided a useful technique to solve the source apportionment of secondary organic particulate matter.
Because there wasn't any analytical technique for directly measuring SOC concentrations, several indirect methods have been applied to estimate SOC. However, each indirect method had its own limitation, and it was hard to quantify SOC. And due to lack of standard carbon analysis method (especially defining the deviding point of OC and EC), different carbon analysis methods gave in different OC and EC concentrations. In this paper, the results of carbon species measured by elemental analysis (EA) method and thermal-optical reflection (TOR) method were compared. The uncertainties of SOC estimation caused by carbon analysis method had been discussed. Based on the relationship of measurement results obtained from these two methods, we put forward an idea about that the content of organic pyrolyzed carbon (OP) obtained from TOR method might be applied to revise the OC concentration measured from EA method.
The modified CMB model was applied to source apportionment of Kaifeng, Wuxi and Panzhihua city. The comparisons of results calculated from modified CMB and traditional CMB model were also conducted, and showed that the source contributions of modified CMB model were more reasonable than that calculated from traditional CMB model.
本论文针对SOC源成分谱难以确定的难题开展研究,提出了采用OC/EC最小比值法来估算受体颗粒物中SOC的浓度,在此基础上,重新构建受体成分谱,使碳组分在受体和源之间更加匹配,建立了修正的CMB模型方程,有效地解决了二次污染物SOC对CMB模型的影响,也为解决二次颗粒物的源解析提供了可借鉴的技术方法。
针对SOC定量困难及目前缺乏碳分析方法的统一标准(尤其是OC、EC的界定)等问题,本研究对同一样品中的碳组分同步采用元素分析(EA)法和热-光碳反射(TOR)法进行测定,结合两类分析方法的原理,对测量结果进行了比较研究,对因分析方法不同造成的SOC定量的不确定性进行了讨论。提出了有可能可以利用TOR法加热过程中得到的OP含量值校正EA法测得的OC浓度的思想。
利用本论文所建立的方法,对开封、无锡和攀枝花三城市的颗粒物进行了来源解析,并与传统的CMB模型结果进行了比较,结果表明,本论文所建立的源解析方法的结果优于传统CMB模型的结果。
The chemical mass balance (CMB) model, which is based on the principle of mass conservation, is one of several receptor models that have been applied to source apportionment of ambient particulate matter, and has been widely used. However, the presence of secondary organic carbon (SOC) brought uncertainties to the results of source apportionment. SOC, which is formed through atmospheric oxidation of volatile organic compounds, isn't emitted directly from primary sources. It was very difficult to identify the SOC source profile for CMB model. Therefore, SOC made the matching degree of carbon species between identified sources and receptor decreased, and resulted in the source contributions calculated from CMB model had larger uncertainties. SOC, which influenced the reliability of CMB model, has been a difficult problem for a long time.
In this study, we focused on the problem that SOC source profile was difficult to be obtained, and put forward a new method to solve this problem. The content of this method included:Using "OC/EC minimum ratio" method to estimate SOC concentration, reconstructing new receptor profile based on SOC concentration, and modifiying CMB model. New receptor profile made carbon species in receptor match well with those in identified sources. This method reduced the influence of SOC on CMB model results, and provided a useful technique to solve the source apportionment of secondary organic particulate matter.
Because there wasn't any analytical technique for directly measuring SOC concentrations, several indirect methods have been applied to estimate SOC. However, each indirect method had its own limitation, and it was hard to quantify SOC. And due to lack of standard carbon analysis method (especially defining the deviding point of OC and EC), different carbon analysis methods gave in different OC and EC concentrations. In this paper, the results of carbon species measured by elemental analysis (EA) method and thermal-optical reflection (TOR) method were compared. The uncertainties of SOC estimation caused by carbon analysis method had been discussed. Based on the relationship of measurement results obtained from these two methods, we put forward an idea about that the content of organic pyrolyzed carbon (OP) obtained from TOR method might be applied to revise the OC concentration measured from EA method.
The modified CMB model was applied to source apportionment of Kaifeng, Wuxi and Panzhihua city. The comparisons of results calculated from modified CMB and traditional CMB model were also conducted, and showed that the source contributions of modified CMB model were more reasonable than that calculated from traditional CMB model.
引文
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