杭州市空气中PAHs的污染特征及源汇机制
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摘要
多环芳烃(PAHs)是一类环境中普遍存在并具有“三致”效应的持久性有机污染物，主要来自化石燃料等不完全燃烧。准确掌握空气中PAHs的浓度水平、污染特征及迁移可为有效控制其污染、保障人群健康提供科学依据。本文以杭州市为代表，研究了公共场所、居民室内空气中PAHs的浓度水平、形态和粒径分布及健康风险，探明了香烟烟雾、卫生球挥发、蜡烛烟雾、秸秆烟气等典型污染源PAHs的排放系数和成分谱图，讨论了不同功能区干、湿沉降中PAHs分布特征，估算了杭州市PAHs的干、湿沉降通量。论文取得了一些有价值的研究成果：
1．探明了典型公共场所室内空气中PAHs的污染特征。春、夏季，商场、超市、车站、酒店、寺庙内15种PAHs总浓度为1．55-36．5μg／m~3。PAHs主要以气态存在，占总浓度的98±1．4％；颗粒态PAHs主要富集在PM_(2．5)上，占颗粒态浓度的71．3±10．1％，其次是PM_(2．5-10)和PM_(＞10)部分，分别占颗粒态浓度的17．6±9．1％和11．1±5．8％。毒性当量浓度计算表明，公共场所内萘(NA)是对人体健康风险贡献最大的PAHs，平均占总风险量的62．4％；气态PAHs对人体健康风险的贡献平均占总风险量的79．3％，PM_(2．5)、PM_(2．5-10)、PM_(＞10)部分的健康风险贡献分别占总风险量的18．4％、1．4％、0．9％。
2．探讨了居民室内空气中PAHs的浓度水平、来源及贡献。夏、冬季，居民室内16种PAHs的总浓度为0．425-36．2μg／m~3，夏季PAHs浓度是冬季的1．5-14．6倍。不同房间内PAHs浓度大小：厨房＞卧室＞书房＞客厅。抽烟家庭室内的PAHs平均总浓度是非抽烟家庭的2．3倍。在非抽烟家庭，卫生球挥发、烹调和未知因素(背景值)是室内PAHs的源，同时室内向室外输出部分PAHs，它们对室内PAHs总浓度的贡献分别为71．5±2．2％、32．8±21．4％、6．2±2．0％和-10．5±2．5％。
3．探明了典型PAHs污染源的排放系数和成分图谱。12种香烟燃烧时16种PAHs平均生成量为6109 ng／cig。9种卫生球中NA的含量为nd-255μg／g，PHEN、AN、PY、AC、FLUOR检出率较高。5种蜡烛燃烧时PAHs生成量为101-141μg／kg。水稻秆和大豆秆焚烧时PAHs的生成量分别为14．4-16．1μg／g和4．57-10．7μg／g。NA是香烟烟雾、蜡烛烟雾和秸秆烟气中主要的PAHs，分别占总浓度的40．2％、76．0％、35．1％。上述3种污染源中3环PAHs所占总浓度的比例分别为35．3％、1 7．7％、46．5％。
4．初步研究了湿沉降中PAHs的来源，并估算了杭州市区PAHs的干、湿沉降通量。相关性分析表明，雨雪中PAHs主要来自空气颗粒物。杭州市区PAHs的干沉降通量为233 kg／yr，湿沉降通量为462 kg／yr。
Polycyclic aromatic hydrocarbons (PAHs)are a kind of widespread persistentorganic pollutants in environment.They are mainly from the uncompletedcombustion of organics,and have the carcinogenic property to humans.In order tocontrol PAH pollution in air efficiently,it is necessary to obtain the occurrences,sources and sinks for PAHs in air.In the dissertation,pollution level,phasedistribution,health risk and influence of life styles for PAHs in indoor (includingpublic places and residential homes)air in Hangzhou were investigated.Emissionamounts and fingerprints of the typical PAH sources such as cigarette smoke,mothball,candle smoke and straw smoke were studied.Furthermore,patterns andsources of PAHs in dry and wet deposition including dust,rain and snow werediscussed,and PAH deposition fluxes in Hangzhou were estimated.The mainconclusions of the dissertation were as follows:
1.Concentrations of 15 PAHs in air of public place such as shopping center,supermarket,station,hotel and temple were 1.55-36.5μg/m~3 in spring and summer.PAHs were mainly in vapor phase (98±1.4%),and particulate PAHs mainlydistributed on PM_(2.5),which accounted for 71.3±10.1% of total particulate phase,andfollowed by PM_(2.5-10)fraction (17.6±9.1%)and PM＞10 fraction (11.1±5.8%).Naphthalene (NA)was the largest contributor to the total health risks associatedwith the inhalation of PAHs (62.4%).In addition,the average contribution of vaporphase,PM_(2.5)fraction,PM_(2.5-10)fraction and PM＞10 fraction to total health risks were79.3%,18.4%,1.4% and 0.9%,respectively.
2.Concentrations of 16 PAHs in residential air were 0.425-36.2μg/m~3 insummer and winter.The ratios of total PAH concentrations in summer to those inwinter were 1.5-14.6.PAH pollution levels:kitchen＞bedroom＞work room＞living room.Concentrations of total PAHs in smoking residential air were 2.3 timeshigher than those in nonsmoking residential air.In nonsmoking residences,mothballemission,cooking practice and unknown source (may be background concentrations)were the sources of indoor PAHs,however outdoor environment was the fate ofindoor PAHs,and they accounted for 71.5±2.2%,32.8±21.4%,6.2±2.0% and-10.5±2.5% of PAHs in residential air,respectively.
3.Emission amounts,influence factors and fingerprints of the typical PAHsources were studied.Emission amounts of 16 PAHs in cigarette smoke,candlesmoke,rice and bean straw smoke were 6109 ng/cig,101-141μg/kg,14.4-16.1μg/gand 4.57-10.7μg/g,respectively.Concentrations of NA in mothball were nd-255 μg/g.NA was the most abundant one in cigarette smoke,candle smoke and strawsmoke,which accounted for 40.2%,76.0% and 35.1% of total PAH concentrations,respectively.3-ring PAHs accounted for 35.3%,17.7% and 46.5% of total PAHconcentrations in these sources,respectively.
4.PAHs in rain and snow were mainly from the particles in air.The estimateddry and wet deposition fluxes of PAHs in Hangzhou were 233 kg/yr and 462 kg/yr,respcetively.
1．探明了典型公共场所室内空气中PAHs的污染特征。春、夏季，商场、超市、车站、酒店、寺庙内15种PAHs总浓度为1．55-36．5μg／m~3。PAHs主要以气态存在，占总浓度的98±1．4％；颗粒态PAHs主要富集在PM_(2．5)上，占颗粒态浓度的71．3±10．1％，其次是PM_(2．5-10)和PM_(＞10)部分，分别占颗粒态浓度的17．6±9．1％和11．1±5．8％。毒性当量浓度计算表明，公共场所内萘(NA)是对人体健康风险贡献最大的PAHs，平均占总风险量的62．4％；气态PAHs对人体健康风险的贡献平均占总风险量的79．3％，PM_(2．5)、PM_(2．5-10)、PM_(＞10)部分的健康风险贡献分别占总风险量的18．4％、1．4％、0．9％。
2．探讨了居民室内空气中PAHs的浓度水平、来源及贡献。夏、冬季，居民室内16种PAHs的总浓度为0．425-36．2μg／m~3，夏季PAHs浓度是冬季的1．5-14．6倍。不同房间内PAHs浓度大小：厨房＞卧室＞书房＞客厅。抽烟家庭室内的PAHs平均总浓度是非抽烟家庭的2．3倍。在非抽烟家庭，卫生球挥发、烹调和未知因素(背景值)是室内PAHs的源，同时室内向室外输出部分PAHs，它们对室内PAHs总浓度的贡献分别为71．5±2．2％、32．8±21．4％、6．2±2．0％和-10．5±2．5％。
3．探明了典型PAHs污染源的排放系数和成分图谱。12种香烟燃烧时16种PAHs平均生成量为6109 ng／cig。9种卫生球中NA的含量为nd-255μg／g，PHEN、AN、PY、AC、FLUOR检出率较高。5种蜡烛燃烧时PAHs生成量为101-141μg／kg。水稻秆和大豆秆焚烧时PAHs的生成量分别为14．4-16．1μg／g和4．57-10．7μg／g。NA是香烟烟雾、蜡烛烟雾和秸秆烟气中主要的PAHs，分别占总浓度的40．2％、76．0％、35．1％。上述3种污染源中3环PAHs所占总浓度的比例分别为35．3％、1 7．7％、46．5％。
4．初步研究了湿沉降中PAHs的来源，并估算了杭州市区PAHs的干、湿沉降通量。相关性分析表明，雨雪中PAHs主要来自空气颗粒物。杭州市区PAHs的干沉降通量为233 kg／yr，湿沉降通量为462 kg／yr。
Polycyclic aromatic hydrocarbons (PAHs)are a kind of widespread persistentorganic pollutants in environment.They are mainly from the uncompletedcombustion of organics,and have the carcinogenic property to humans.In order tocontrol PAH pollution in air efficiently,it is necessary to obtain the occurrences,sources and sinks for PAHs in air.In the dissertation,pollution level,phasedistribution,health risk and influence of life styles for PAHs in indoor (includingpublic places and residential homes)air in Hangzhou were investigated.Emissionamounts and fingerprints of the typical PAH sources such as cigarette smoke,mothball,candle smoke and straw smoke were studied.Furthermore,patterns andsources of PAHs in dry and wet deposition including dust,rain and snow werediscussed,and PAH deposition fluxes in Hangzhou were estimated.The mainconclusions of the dissertation were as follows:
1.Concentrations of 15 PAHs in air of public place such as shopping center,supermarket,station,hotel and temple were 1.55-36.5μg/m~3 in spring and summer.PAHs were mainly in vapor phase (98±1.4%),and particulate PAHs mainlydistributed on PM_(2.5),which accounted for 71.3±10.1% of total particulate phase,andfollowed by PM_(2.5-10)fraction (17.6±9.1%)and PM＞10 fraction (11.1±5.8%).Naphthalene (NA)was the largest contributor to the total health risks associatedwith the inhalation of PAHs (62.4%).In addition,the average contribution of vaporphase,PM_(2.5)fraction,PM_(2.5-10)fraction and PM＞10 fraction to total health risks were79.3%,18.4%,1.4% and 0.9%,respectively.
2.Concentrations of 16 PAHs in residential air were 0.425-36.2μg/m~3 insummer and winter.The ratios of total PAH concentrations in summer to those inwinter were 1.5-14.6.PAH pollution levels:kitchen＞bedroom＞work room＞living room.Concentrations of total PAHs in smoking residential air were 2.3 timeshigher than those in nonsmoking residential air.In nonsmoking residences,mothballemission,cooking practice and unknown source (may be background concentrations)were the sources of indoor PAHs,however outdoor environment was the fate ofindoor PAHs,and they accounted for 71.5±2.2%,32.8±21.4%,6.2±2.0% and-10.5±2.5% of PAHs in residential air,respectively.
3.Emission amounts,influence factors and fingerprints of the typical PAHsources were studied.Emission amounts of 16 PAHs in cigarette smoke,candlesmoke,rice and bean straw smoke were 6109 ng/cig,101-141μg/kg,14.4-16.1μg/gand 4.57-10.7μg/g,respectively.Concentrations of NA in mothball were nd-255 μg/g.NA was the most abundant one in cigarette smoke,candle smoke and strawsmoke,which accounted for 40.2%,76.0% and 35.1% of total PAH concentrations,respectively.3-ring PAHs accounted for 35.3%,17.7% and 46.5% of total PAHconcentrations in these sources,respectively.
4.PAHs in rain and snow were mainly from the particles in air.The estimateddry and wet deposition fluxes of PAHs in Hangzhou were 233 kg/yr and 462 kg/yr,respcetively.
引文
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