济南市大气PM_（2.5）污染特征、来源解析及其对能见度的影响
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摘要
为了查明山东省省会—济南市PM_(2.5)的污染特征,自2004年11月-2005年9月及2006年2月-2007年2月,利用PM_(2.5)四通道采样仪、PM_(2.5)/PM_(10)双通道采样仪、MOUDI多级采样仪、离子色谱、C/H/O元素分析仪及X射线荧光等研究手段,对济南市PM_(2.5)的浓度水平、化学组成、来源、气象条件对PM_(2.5)污染水平的影响及PM_(2.5)对能见度的影响进行了系统的研究。得到了如下有意义的结论:
1.济南市PM_(2.5)污染严重且市区PM_(2.5)的污染况比郊区严重。山大点和苗圃点PM_(2.5)日均浓度分别超出美国EPA的日均值标准(35μg/m~3)2.98和1.79倍。水溶性离子是济南市PM_(2.5)中所占比例最大的组分,其中SO_4~(2-)、NO_3~-及NH_4~+是最主要的水溶性离子。在济南市PM_(2.5)体系中均以(NH_4)_2SO_4和NH_4NO_3形式存在。碳质组分(OC+EC)是济南市PM_(2.5)中所占比例为第二位的组分。济南市大气PM_(2.5)中有机物和二次污染十分严重,呈现出复合型污染的特征。
2.山东地区冬季受蒙古高压的影响;其它季节由于受华北地形槽的影响,在东经115°附近存在一个东北-西南走向的辐合带,该辐合带的来回移动导致山东地区的污染物不易扩散,污染物浓度高。当大气流场为西北气流型、辐合气流型及反气旋气流型时,易导致PM_(2.5)高浓度污染。
3.利用多元线性回归模型对PM_(2.5)浓度进行模拟,模拟的结果较实测值有所偏低,当PM_(2.5)的浓度质量浓度小于200μg/m~3时,模拟的结果比较好,当PM_(2.5)的质量浓度大于200μg/m~3时,模拟结果不好。浓度取对数时,模拟的结果比直接取浓度值得到的结果要好。
4.济南市能见度自1961-2005整体呈下降趋势,颗粒物污染和气象条件对能见度下降的贡献相当。能见度和PM_(2.5)及PM_(10)浓度均呈指数关系且能见度和PM_(2.5)的相关性高于与PM_(10)的相关性。硫酸盐是PM_(2.5)中对能见度下降贡献最大的成分,二次气溶胶(NH_4)_2SO_4,NH_4NO_3,POM))对能见度下降的贡献高于一次颗粒物BC。灰霾天TSP,PM_(10)和PM_(1.8)的浓度明显高于晴朗天气条件下。灰霾天气条件下,细颗粒物比例增加,水溶性离子主要富集在细模态中,灰霾天有利于SO_4~(2-)和NO_3~-和二次有机气溶胶的形成。
5.济南市市区及郊区PM_(2.5)主要来源及年均贡献无明显差异,其来源依次为:道路扬尘和机动车尾气(15.0-16.0%)、工业排放源(15.1-17.5%)、燃煤(13.6-18.7%)、土壤尘源(19.0-22.8%)、二次源(19.5-20.0%)、生物质燃烧(17.7%)。
To investigate the characteristics of the fine particle matter in Jinan,PM_(2.5)samples were collected by two/four channel and MOUDI sampler from February 2007 to September 2005.The samples were analyzed by IC,C/H/O,XRF and so on.The chemical characteristics of the fine particle matter and source appointments were studied in detail.Furthermore,the impact of meteorological conditions on PM_(2.5)level and the influence of PM_(2.5)on visibility were also carefully investigated.The results were obtained as follows:
1.PM_(2.5)pollution in Jinan is serious and PM_(2.5)pollution of urban is more serious than suburban.The daily PM_(2.5)concentrations of Shandong University and Miaopu station exceed US EPA daily average standard(35μg/m~3)of 2.98 and 1.79 times. Water-soluble ions in Jinan account for the largest proportion in PM_(2.5)components. While,SO_4~(2-),NO_3~+ and NH_4~+ are the most important water-soluble ions.The form of above three ions are(NH_4)_2SO_4 and NH_4NO_3.Carbonaceous components(OC + EC) are the second largest proportion.The organic compounds and secondary pollution in the atmosphere are very serious,showing compound pollution characteristics.
2.Winter is affected by Mongolia hypertension in Shandong.While,other season is due to the impact of the North China terrain trough in the vicinity.There is a Northeast - Southwest Composite Strip in longitude 115°,the return to movement of Composite Strip in Shandong could hinder the diffusion of pollutants.When fild-flow is the Northwest,convergent flow of air and anti-cyclone type,it favorite high concentrations of PM_(2.5)pollution.
3.Using multiple linear regression models to simulate the PM_(2.5)concentrations, the results of simulations is relatively lower than experimental data.When the concentration of PM_(2.5)is more than 200μg/m~3,simulation results is good,and when PM_(2.5)concentration is less than 200μg/m~3,the simulation method does not work well. From the concentrations of Log,the results of simulations are better than directly from the concentration.
4.The visual range in Jinan showed a general decreasing trend from 1961 to 2005. Meteorological conditions and particulate matter made comparable contributions to the decrease of visual range in Jinan.In every season,the visual range accorded well with the concentrations of PM_2.5)and PM_(10)in an exponential relationship and showed a higher correlation with PM_(2.5)than PM_(10).Sulfate is the largest contributor to visual range degradation The results demonstrate that secondary particulate matter((NH_4)_2SO_4, NH_4NO_3,POM)contributed much more to the decrease of visual range in Jinan than primary particles(BC).Long-range transport of air masses from the north(including northwest and northeast)of Jinan and from the ocean,carrying high concentrations of secondary aerosol(SO_4~(2-),NH_4~+,NO_3~-)combined with weather conditions of high relative and low wind speed can make contributions to the formation of hazy days in winter and summer respectively.
5.The main source of PM_(2.5)and annual contribution is no obviously different between Jinan City and the suburban.Their sources were:road dust and vehicle exhaust (15.0-16.0%),industrial sources of emissions(15.1-17.5%),coal(13.6 -18.7%),soil dust(19.0-22.8%),secondary sources(19.5-20.0%),biomass burning(17.7%).
1.济南市PM_(2.5)污染严重且市区PM_(2.5)的污染况比郊区严重。山大点和苗圃点PM_(2.5)日均浓度分别超出美国EPA的日均值标准(35μg/m~3)2.98和1.79倍。水溶性离子是济南市PM_(2.5)中所占比例最大的组分,其中SO_4~(2-)、NO_3~-及NH_4~+是最主要的水溶性离子。在济南市PM_(2.5)体系中均以(NH_4)_2SO_4和NH_4NO_3形式存在。碳质组分(OC+EC)是济南市PM_(2.5)中所占比例为第二位的组分。济南市大气PM_(2.5)中有机物和二次污染十分严重,呈现出复合型污染的特征。
2.山东地区冬季受蒙古高压的影响;其它季节由于受华北地形槽的影响,在东经115°附近存在一个东北-西南走向的辐合带,该辐合带的来回移动导致山东地区的污染物不易扩散,污染物浓度高。当大气流场为西北气流型、辐合气流型及反气旋气流型时,易导致PM_(2.5)高浓度污染。
3.利用多元线性回归模型对PM_(2.5)浓度进行模拟,模拟的结果较实测值有所偏低,当PM_(2.5)的浓度质量浓度小于200μg/m~3时,模拟的结果比较好,当PM_(2.5)的质量浓度大于200μg/m~3时,模拟结果不好。浓度取对数时,模拟的结果比直接取浓度值得到的结果要好。
4.济南市能见度自1961-2005整体呈下降趋势,颗粒物污染和气象条件对能见度下降的贡献相当。能见度和PM_(2.5)及PM_(10)浓度均呈指数关系且能见度和PM_(2.5)的相关性高于与PM_(10)的相关性。硫酸盐是PM_(2.5)中对能见度下降贡献最大的成分,二次气溶胶(NH_4)_2SO_4,NH_4NO_3,POM))对能见度下降的贡献高于一次颗粒物BC。灰霾天TSP,PM_(10)和PM_(1.8)的浓度明显高于晴朗天气条件下。灰霾天气条件下,细颗粒物比例增加,水溶性离子主要富集在细模态中,灰霾天有利于SO_4~(2-)和NO_3~-和二次有机气溶胶的形成。
5.济南市市区及郊区PM_(2.5)主要来源及年均贡献无明显差异,其来源依次为:道路扬尘和机动车尾气(15.0-16.0%)、工业排放源(15.1-17.5%)、燃煤(13.6-18.7%)、土壤尘源(19.0-22.8%)、二次源(19.5-20.0%)、生物质燃烧(17.7%)。
To investigate the characteristics of the fine particle matter in Jinan,PM_(2.5)samples were collected by two/four channel and MOUDI sampler from February 2007 to September 2005.The samples were analyzed by IC,C/H/O,XRF and so on.The chemical characteristics of the fine particle matter and source appointments were studied in detail.Furthermore,the impact of meteorological conditions on PM_(2.5)level and the influence of PM_(2.5)on visibility were also carefully investigated.The results were obtained as follows:
1.PM_(2.5)pollution in Jinan is serious and PM_(2.5)pollution of urban is more serious than suburban.The daily PM_(2.5)concentrations of Shandong University and Miaopu station exceed US EPA daily average standard(35μg/m~3)of 2.98 and 1.79 times. Water-soluble ions in Jinan account for the largest proportion in PM_(2.5)components. While,SO_4~(2-),NO_3~+ and NH_4~+ are the most important water-soluble ions.The form of above three ions are(NH_4)_2SO_4 and NH_4NO_3.Carbonaceous components(OC + EC) are the second largest proportion.The organic compounds and secondary pollution in the atmosphere are very serious,showing compound pollution characteristics.
2.Winter is affected by Mongolia hypertension in Shandong.While,other season is due to the impact of the North China terrain trough in the vicinity.There is a Northeast - Southwest Composite Strip in longitude 115°,the return to movement of Composite Strip in Shandong could hinder the diffusion of pollutants.When fild-flow is the Northwest,convergent flow of air and anti-cyclone type,it favorite high concentrations of PM_(2.5)pollution.
3.Using multiple linear regression models to simulate the PM_(2.5)concentrations, the results of simulations is relatively lower than experimental data.When the concentration of PM_(2.5)is more than 200μg/m~3,simulation results is good,and when PM_(2.5)concentration is less than 200μg/m~3,the simulation method does not work well. From the concentrations of Log,the results of simulations are better than directly from the concentration.
4.The visual range in Jinan showed a general decreasing trend from 1961 to 2005. Meteorological conditions and particulate matter made comparable contributions to the decrease of visual range in Jinan.In every season,the visual range accorded well with the concentrations of PM_2.5)and PM_(10)in an exponential relationship and showed a higher correlation with PM_(2.5)than PM_(10).Sulfate is the largest contributor to visual range degradation The results demonstrate that secondary particulate matter((NH_4)_2SO_4, NH_4NO_3,POM)contributed much more to the decrease of visual range in Jinan than primary particles(BC).Long-range transport of air masses from the north(including northwest and northeast)of Jinan and from the ocean,carrying high concentrations of secondary aerosol(SO_4~(2-),NH_4~+,NO_3~-)combined with weather conditions of high relative and low wind speed can make contributions to the formation of hazy days in winter and summer respectively.
5.The main source of PM_(2.5)and annual contribution is no obviously different between Jinan City and the suburban.Their sources were:road dust and vehicle exhaust (15.0-16.0%),industrial sources of emissions(15.1-17.5%),coal(13.6 -18.7%),soil dust(19.0-22.8%),secondary sources(19.5-20.0%),biomass burning(17.7%).
引文
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