大气污染源排放颗粒物组成、有害组分风险评价及清单构建研究
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摘要
源排放颗粒物的组成是受体模型解析大气颗粒物来源的基础。对源排放颗粒物的组成了解越详尽准确，大气颗粒物来源的判断结果就越准确可靠。目前国内外源成分谱缺乏且陈旧，源特征标识组分等相关信息极度匮乏，尤其是受采样条件的限制，现有的燃烧源成分谱大多不能代表其真实排放。当前燃烧源排放有毒有害空气污染物的环境影响已成为国内外研究的热点，而源排放清单不确定性的一个重要因素在于排放因子的不确定性，尤其是国内相关研究多借鉴国外的排放因子，并不能反应国内的真实排放水平。采用能真实反应大气颗粒物污染源排放颗粒物的采样设备，对大气主要污染源排放不同粒径的颗粒物上化学组分的排放浓度、百分含量组成、标识组分、排放因子等进行研究具有重要的科学和现实意义。
本文通过再悬浮采样方法建立了土壤尘、道路尘和城市扬尘三种开放源排放TSP/PM_(10)/PM_(2.5)上载带的无机组分和PAHs成分谱，比较不同粒径颗粒上组分含量、成分谱组成、标识组分特征比值等之间的差异，为大气颗粒物来源解析提供精准的基础数据，并对三种粒径尘载带重金属和PAHs的来源的环境和人体健康风险进行了评价；利用自行设计的二级稀释通道采样器建立了固定源排放PM_(10)和PM_(2.5)两种粒径载带无机组分和PAHs成分谱和有害组分（碳组分、重金属和PAHs）排放因子，比较了成分谱的差异、获得了PAHs标识组分、更新和完善了PAHs特征比值及特征元素比值；利用二级稀释通道采样器和便携式机动车尾气采样系统，通过发动机台架实验研究工况对轻型和重型柴油发动机排放颗粒物上化学组分的影响，系统地研究了11工况下轻型/重型柴油发动机排放PM_(10)/PM_(2.5)载带组分成分谱和排放因子，研究发动机运行参数对其排放颗粒上组分的影响；并通过道路随车采样，获得了机动车在真实路况上行驶时排放PM_(10)/PM_(2.5)载带无机组分和PAHs含量、成分谱组成和有害组分排放因子，并比较不同类型、不同运行时段、不同负载、不同燃料类型的机动车排放颗粒物上化学组分的差异；利用稀释通道采样器，系统地研究了家庭炉灶燃烧玉米秸秆、木材、蜂窝煤、块煤排放PM_(10)/PM_(2.5)载带无机组分和PAHs含量、成分谱组成和有害组分排放因子。本研究将国内相关领域首次带入到细颗粒水平；从源的角度分析了阴阳离子比值、NO_3~-/SO_4~(2-)和OC/EC比值，这些工作可为大气颗粒物酸缓冲能力分析、颗粒物来源解析、二次碳气溶胶来源判断等提供可靠源数据支撑，也将会带动有关研究者重新审视这些领域的研究；并利用实测所得燃烧源排放PM_(2.5)上有害组分的排放因子，结合能源统计年鉴、农业统计年鉴等相关信息，建立我国2009-2010年各燃烧源排放PM_(2.5)中相应组分的源排放清单，在国内外首次将排放清单的研究深入到细颗粒组分层面。
本文的主要结论为：（1）再悬浮采样方法为当前研究开放源排放颗粒物中不同粒径颗粒化学组分的有效方法，稀释通道采样方法为获得燃烧源排放粗细颗粒物中化学组分的有效方法，现有的稀释通道采样设备需要进一步完善和推广，以满足大气颗粒物污染源监测与表征的需要；（2）燃烧源排放PM_(2.5)和PM_(10)的质量浓度在0.21-503.3mg/m3和0.41-869.2mg/m3之间，室内块煤燃烧排放颗粒的质量浓度最高；（3）燃烧源排放PM_(2.5)和PM_(10)中浓度较高的几种组分通常为Al、Ca、Fe、Si、NO_3~-、SO_4~(2-)、OC和EC等，不同类型的源排放颗粒物中这些组分的差异较大；（4）阴阳离子的当量浓度比值分析表明大多数燃烧源排放的颗粒为酸性，除秸秆燃烧和柴油卡车排放颗粒物有时会表现为碱性；（5）燃烧源排放颗粒中NO_3~-/SO_4~(2-)比值均小于1，OC/EC比值在多数情况下也远大于2。在大气颗粒物来源解析中用NO_3~-/SO_4~(2-)判断机动车尾气和固定燃烧源对于大气颗粒物的影响的重要程度和用OC/EC大于2来判断大气二次气溶胶存在时应慎重；（6）不同类型燃烧源排放PM_(2.5)和PM_(10)中特征元素比值Cu/Sb、As/V、Ni/V、Zn/Pb和Zn/Cd的比值差异较大，在应用于来源解析时，应尽可能的采用某一地区的源排放数据，且需考虑到粒径的差异；（7）分歧系数表明大多数燃烧源排放颗粒物的成分谱均存在差异，尤其是针对细颗粒物；（8）不同类型燃烧源排放粗细颗粒中PAHs的质量浓度变化范围差异较大，优势组分含量、环数分布、组分百分含量组成、毒性、PAHs标识组分、特征比值等也随源类型和颗粒粒径的不同差异很大。在应用于大气颗粒物中PAHs来源解析判断时，需尽可能的采用当地的源排放数据，同时现有的PAHs源排放成分谱、排放因子、特征比值等也需要不断完善和及时更新；（9）本研究得到了六种固定源、六种类型机动车、四种室内燃料排放PM_(2.5)和PM_(10)两种粒径上OC、EC、V、Cr、Mn、Co、Ni、Cu、Zn、As、Cd、Sb、Pb和PAHs排放因子和排放因子的不确定度，可为当前我国空气中有毒有害污染物排放清单提供基础数据。
Chemical compositions of particulate matter (PM) emitted from atmosphericpollution sources are the base of receptor models. The more specific and accuracy ofthe source characteristic, the more reliable source apportionment results foratmospheric PM could be obtained. Now the data about source profiles were out ofdate and the information associated with source markers was still limited. The reasonlied on the limitation of source sampling methods. Current source profiles for PMmostly can not reflect the real emission of combustion sources to the atmosphere.Recently, the impact of hazardous and toxic air pollutants emitted from combustionsources on the environment received wide attention. The emission factors (EFs) datais one of key factors for the accuracy of corresponding emission inventories. For thestudies in China, the EFs were mostly referred to foreign literatures which may biasthe emission inventory results. Therefore, adopting the sampling system which couldcollect the real PM to be emitted into the air and obtaining the emissionconcentrations, mass percentages, source markers, emission factors, etc of chemicalcomponents in PM are of significant scientific and practical meaning.
Firstly, this study established the inorganic chemical components and PAHsprofiles for TSP, PM_(10)and PM_(2.5)fractions of soil dust, road dust and resuspended dust.The contents of chemical species, profile composition, markers and specific elementaland PAHs ratios were compared among different size of particles and different typesof dust. Results obtained here could be used in other source apportionment studies.Meanwhile, the environment and human health risks related with heavy meatls andPAHs in dusts were assessed. Secondly, the paper obtained inorganic chemicalcomponents and PAHs profiles for PM_(10)and PM_(2.5)fractions of stationary sourceswith dilution sampling system. The contents of chemical species, profile composition,markers and specific elemental and PAHs ratios were updated. Thirdly, by dilutionsampling system, this research also studied the inorganic chemical components andPAHs profiles for PM_(10)and PM_(2.5)fractions of two diesel engines and obtained theinfluence of engine operating paramaters on the emission of chemical components.Then the contents of chemical species, profile composition, markers and specificelemental and PAHs ratios of PM_(10)and PM_(2.5)emitted from vehicles running on realroad with different loads, fuel types, running time scales and vehicle types were investigated. Fourthly, the contents of chemical species, profile composition, markersand specific elemental and PAHs ratios of PM_(10)and PM_(2.5)emitted from straw, wood,honey coal and raw coal burning were detected. At each section, we analyzed theanion/cation, NO_3~-/SO_4~(2-)and OC/EC ratios which may stimulate related studies incorresponding fields like the analysis of acid-neutralization ability of PM, sourceapportionment of PM and source identification of secondary carbonic aerosol. At last,according to self-detected EFs for carbonic components, heavy metals and PAHs andinformation about activity levels, this paper established the emission inventories forthese hazardous species in PM_(2.5)for the year of2009or2010in China. This is thefirst study which established emission inventories for the species in PM_(2.5).
The main conclusions were:(1) resuspension chamber sampling and dilutionsampling were the effective methods to study fugitive dust and combustion sourcesrespectively which should be improved and used more widely in other studies;(2) themass concentrations of PM_(2.5)and PM_(10)emitted from combustion sources were0.21-503.3mg/m3and0.41-869.2mg/m3, with the highest concentrations for domesticraw coal combustion;(3) Al, Ca, Fe, Si, NO_3~-, SO_4~(2-), OC and EC were always theabundant species for combustion sources and there existed diversities of the contentsfor them from different sources;(4) the anion/cation ratio analysis indicated PMemitted from most combustion sources were acid, excepted for the PM from cornstraw burning and several running situations for diesel cars;(5) the NO_3~-/SO_4~(2-)ratioswere always less than1and the OC/EC values were always higher than2for PMemitted from combustion sources. Therefore, to identify the importance of stationarysources and vehicle emission for atmospheric PM, the NO_3~-/SO_4~(2-)ratio should be usedwith caution. It is the same for adopting OC/EC>2to identify the existence ofsecondary carbonic aerosol;(6) specific elemental ratios-Cu/Sb、As/V、Ni/V、Zn/Pband Zn/Cd exhibited obvious difference for different types of combustion sources andbetween the two fractions of particles, so local data should be used in sourceapportionment studies and the diversities between size of particles should also beconsidered;(7) coefficient of divergence values implied that source profiles of PMwere different for various combustion sources, especially for the fine particles. Localsources profiles of PM should be established and updated timely;(8) the massconcentrations of PAHs, the contents of abundant PAHs, ring distribution, toxicity,markers, specific PAHs ratios, etc in PM_(10)and PM_(2.5)were different for varioussources and the two size of particles. All these data are needed to be established and updated timely;(9) the EFs for OC, EC, V, Cr, Mn, Co, Ni, Cu, Zn, As, Cd, Sb, Pband PAHs in PM_(10)and PM_(2.5)were obtained for six types of stationary sources, sixtypes of vehicles and four kinds of domestic fuels burning and the uncertainty of EFswere analyzed which could be used in establishing emission inventories of hazardousair pollutants for China.
本文通过再悬浮采样方法建立了土壤尘、道路尘和城市扬尘三种开放源排放TSP/PM_(10)/PM_(2.5)上载带的无机组分和PAHs成分谱，比较不同粒径颗粒上组分含量、成分谱组成、标识组分特征比值等之间的差异，为大气颗粒物来源解析提供精准的基础数据，并对三种粒径尘载带重金属和PAHs的来源的环境和人体健康风险进行了评价；利用自行设计的二级稀释通道采样器建立了固定源排放PM_(10)和PM_(2.5)两种粒径载带无机组分和PAHs成分谱和有害组分（碳组分、重金属和PAHs）排放因子，比较了成分谱的差异、获得了PAHs标识组分、更新和完善了PAHs特征比值及特征元素比值；利用二级稀释通道采样器和便携式机动车尾气采样系统，通过发动机台架实验研究工况对轻型和重型柴油发动机排放颗粒物上化学组分的影响，系统地研究了11工况下轻型/重型柴油发动机排放PM_(10)/PM_(2.5)载带组分成分谱和排放因子，研究发动机运行参数对其排放颗粒上组分的影响；并通过道路随车采样，获得了机动车在真实路况上行驶时排放PM_(10)/PM_(2.5)载带无机组分和PAHs含量、成分谱组成和有害组分排放因子，并比较不同类型、不同运行时段、不同负载、不同燃料类型的机动车排放颗粒物上化学组分的差异；利用稀释通道采样器，系统地研究了家庭炉灶燃烧玉米秸秆、木材、蜂窝煤、块煤排放PM_(10)/PM_(2.5)载带无机组分和PAHs含量、成分谱组成和有害组分排放因子。本研究将国内相关领域首次带入到细颗粒水平；从源的角度分析了阴阳离子比值、NO_3~-/SO_4~(2-)和OC/EC比值，这些工作可为大气颗粒物酸缓冲能力分析、颗粒物来源解析、二次碳气溶胶来源判断等提供可靠源数据支撑，也将会带动有关研究者重新审视这些领域的研究；并利用实测所得燃烧源排放PM_(2.5)上有害组分的排放因子，结合能源统计年鉴、农业统计年鉴等相关信息，建立我国2009-2010年各燃烧源排放PM_(2.5)中相应组分的源排放清单，在国内外首次将排放清单的研究深入到细颗粒组分层面。
本文的主要结论为：（1）再悬浮采样方法为当前研究开放源排放颗粒物中不同粒径颗粒化学组分的有效方法，稀释通道采样方法为获得燃烧源排放粗细颗粒物中化学组分的有效方法，现有的稀释通道采样设备需要进一步完善和推广，以满足大气颗粒物污染源监测与表征的需要；（2）燃烧源排放PM_(2.5)和PM_(10)的质量浓度在0.21-503.3mg/m3和0.41-869.2mg/m3之间，室内块煤燃烧排放颗粒的质量浓度最高；（3）燃烧源排放PM_(2.5)和PM_(10)中浓度较高的几种组分通常为Al、Ca、Fe、Si、NO_3~-、SO_4~(2-)、OC和EC等，不同类型的源排放颗粒物中这些组分的差异较大；（4）阴阳离子的当量浓度比值分析表明大多数燃烧源排放的颗粒为酸性，除秸秆燃烧和柴油卡车排放颗粒物有时会表现为碱性；（5）燃烧源排放颗粒中NO_3~-/SO_4~(2-)比值均小于1，OC/EC比值在多数情况下也远大于2。在大气颗粒物来源解析中用NO_3~-/SO_4~(2-)判断机动车尾气和固定燃烧源对于大气颗粒物的影响的重要程度和用OC/EC大于2来判断大气二次气溶胶存在时应慎重；（6）不同类型燃烧源排放PM_(2.5)和PM_(10)中特征元素比值Cu/Sb、As/V、Ni/V、Zn/Pb和Zn/Cd的比值差异较大，在应用于来源解析时，应尽可能的采用某一地区的源排放数据，且需考虑到粒径的差异；（7）分歧系数表明大多数燃烧源排放颗粒物的成分谱均存在差异，尤其是针对细颗粒物；（8）不同类型燃烧源排放粗细颗粒中PAHs的质量浓度变化范围差异较大，优势组分含量、环数分布、组分百分含量组成、毒性、PAHs标识组分、特征比值等也随源类型和颗粒粒径的不同差异很大。在应用于大气颗粒物中PAHs来源解析判断时，需尽可能的采用当地的源排放数据，同时现有的PAHs源排放成分谱、排放因子、特征比值等也需要不断完善和及时更新；（9）本研究得到了六种固定源、六种类型机动车、四种室内燃料排放PM_(2.5)和PM_(10)两种粒径上OC、EC、V、Cr、Mn、Co、Ni、Cu、Zn、As、Cd、Sb、Pb和PAHs排放因子和排放因子的不确定度，可为当前我国空气中有毒有害污染物排放清单提供基础数据。
Chemical compositions of particulate matter (PM) emitted from atmosphericpollution sources are the base of receptor models. The more specific and accuracy ofthe source characteristic, the more reliable source apportionment results foratmospheric PM could be obtained. Now the data about source profiles were out ofdate and the information associated with source markers was still limited. The reasonlied on the limitation of source sampling methods. Current source profiles for PMmostly can not reflect the real emission of combustion sources to the atmosphere.Recently, the impact of hazardous and toxic air pollutants emitted from combustionsources on the environment received wide attention. The emission factors (EFs) datais one of key factors for the accuracy of corresponding emission inventories. For thestudies in China, the EFs were mostly referred to foreign literatures which may biasthe emission inventory results. Therefore, adopting the sampling system which couldcollect the real PM to be emitted into the air and obtaining the emissionconcentrations, mass percentages, source markers, emission factors, etc of chemicalcomponents in PM are of significant scientific and practical meaning.
Firstly, this study established the inorganic chemical components and PAHsprofiles for TSP, PM_(10)and PM_(2.5)fractions of soil dust, road dust and resuspended dust.The contents of chemical species, profile composition, markers and specific elementaland PAHs ratios were compared among different size of particles and different typesof dust. Results obtained here could be used in other source apportionment studies.Meanwhile, the environment and human health risks related with heavy meatls andPAHs in dusts were assessed. Secondly, the paper obtained inorganic chemicalcomponents and PAHs profiles for PM_(10)and PM_(2.5)fractions of stationary sourceswith dilution sampling system. The contents of chemical species, profile composition,markers and specific elemental and PAHs ratios were updated. Thirdly, by dilutionsampling system, this research also studied the inorganic chemical components andPAHs profiles for PM_(10)and PM_(2.5)fractions of two diesel engines and obtained theinfluence of engine operating paramaters on the emission of chemical components.Then the contents of chemical species, profile composition, markers and specificelemental and PAHs ratios of PM_(10)and PM_(2.5)emitted from vehicles running on realroad with different loads, fuel types, running time scales and vehicle types were investigated. Fourthly, the contents of chemical species, profile composition, markersand specific elemental and PAHs ratios of PM_(10)and PM_(2.5)emitted from straw, wood,honey coal and raw coal burning were detected. At each section, we analyzed theanion/cation, NO_3~-/SO_4~(2-)and OC/EC ratios which may stimulate related studies incorresponding fields like the analysis of acid-neutralization ability of PM, sourceapportionment of PM and source identification of secondary carbonic aerosol. At last,according to self-detected EFs for carbonic components, heavy metals and PAHs andinformation about activity levels, this paper established the emission inventories forthese hazardous species in PM_(2.5)for the year of2009or2010in China. This is thefirst study which established emission inventories for the species in PM_(2.5).
The main conclusions were:(1) resuspension chamber sampling and dilutionsampling were the effective methods to study fugitive dust and combustion sourcesrespectively which should be improved and used more widely in other studies;(2) themass concentrations of PM_(2.5)and PM_(10)emitted from combustion sources were0.21-503.3mg/m3and0.41-869.2mg/m3, with the highest concentrations for domesticraw coal combustion;(3) Al, Ca, Fe, Si, NO_3~-, SO_4~(2-), OC and EC were always theabundant species for combustion sources and there existed diversities of the contentsfor them from different sources;(4) the anion/cation ratio analysis indicated PMemitted from most combustion sources were acid, excepted for the PM from cornstraw burning and several running situations for diesel cars;(5) the NO_3~-/SO_4~(2-)ratioswere always less than1and the OC/EC values were always higher than2for PMemitted from combustion sources. Therefore, to identify the importance of stationarysources and vehicle emission for atmospheric PM, the NO_3~-/SO_4~(2-)ratio should be usedwith caution. It is the same for adopting OC/EC>2to identify the existence ofsecondary carbonic aerosol;(6) specific elemental ratios-Cu/Sb、As/V、Ni/V、Zn/Pband Zn/Cd exhibited obvious difference for different types of combustion sources andbetween the two fractions of particles, so local data should be used in sourceapportionment studies and the diversities between size of particles should also beconsidered;(7) coefficient of divergence values implied that source profiles of PMwere different for various combustion sources, especially for the fine particles. Localsources profiles of PM should be established and updated timely;(8) the massconcentrations of PAHs, the contents of abundant PAHs, ring distribution, toxicity,markers, specific PAHs ratios, etc in PM_(10)and PM_(2.5)were different for varioussources and the two size of particles. All these data are needed to be established and updated timely;(9) the EFs for OC, EC, V, Cr, Mn, Co, Ni, Cu, Zn, As, Cd, Sb, Pband PAHs in PM_(10)and PM_(2.5)were obtained for six types of stationary sources, sixtypes of vehicles and four kinds of domestic fuels burning and the uncertainty of EFswere analyzed which could be used in establishing emission inventories of hazardousair pollutants for China.
引文
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