河北省涞水县大气颗粒物单颗粒分析表征及来源识别
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摘要
为了解河北省涞水县颗粒物污染特征,采用单颗粒分析技术扫描电镜-X射线能谱法和气团后向轨迹分析技术对该县2015年3个典型污染时段[即正常管控、严格管控(2015年阅兵期间)及发生严重颗粒物染污]采集的7个大气颗粒物样品进行了分析表征和来源解析.共测量了1 506个粒径≥0.5μm的单颗粒,其中粒径小于2.5μm的颗粒占98%以上,测量结果揭示了细颗粒污染特征.结果表明:(1)碳质颗粒为主要颗粒物种类,其检出数目占比在90%以上.(2)非供暖期严格管控时段,当地居民日常生活产生的球形碳质颗粒检出数目占比最高.(3)非供暖期正常管控时段,机动车排放的碳质集合体颗粒检出数目占比最高,交通污染贡献最大.(4)供暖期球形碳质颗粒检出数目占比最高,含硫颗粒检出数目占比相对增加,燃煤的贡献最大.3个采样时段48 h气团后向轨迹分析结果表明,在空气质量良好、颗粒物污染水平较低的情况下,影响研究区域空气质量的主要是本地源;雾霾天气(处于严重颗粒物污染时段)时,西南方向外来源和本地源共同构成研究区域的颗粒物污染状态.
Laishui County in Hebei Province is located 90 km southwest to Beijing. In order to understand the local pollution characteristics of particulate matter,individual-particle analysis technique(SEM-EDX) was performed on 7 samples of atmospheric particles collected in 3 typical periods of atmosphere pollution in Laishui County. In total 1506 particles(diameter larger than 0. 5 μm)were measured,and the diameter of more than 98% particles was less than 2. 5 μm,indicating a characteristic of severe fine particle pollution. The results show that:(1) Carbonaceous particles are the main types of particulate matter and the number detected is over90%.(2) During the China Military Parade,a non-heating period with strict atmospheric control policies implemented,the spherical carbon-rich particles,which were mainly from daily activities of citizens,had the highest number abundance among all particles.(3) During normal non-heating days,abundance of vehicle-emitted soot aggregates was the highest,which showed the largest contribution of traffic to particle pollution.(4) Abundance of spherical carbon-rich particles was highest during heat-period,while the abundance of S-rich particles was significantly increased,implying the main contribution of coal combustion emission to air pollution. Combined with 48-h analysis of air mass back trajectories in 3 typical periods of atmosphere pollution,it was concluded that the local sources were themain cause of pollutants during periods with low level air pollution,while external and local sources both play an important role during periods with severe air pollution in Laishui County.
Laishui County in Hebei Province is located 90 km southwest to Beijing. In order to understand the local pollution characteristics of particulate matter,individual-particle analysis technique(SEM-EDX) was performed on 7 samples of atmospheric particles collected in 3 typical periods of atmosphere pollution in Laishui County. In total 1506 particles(diameter larger than 0. 5 μm)were measured,and the diameter of more than 98% particles was less than 2. 5 μm,indicating a characteristic of severe fine particle pollution. The results show that:(1) Carbonaceous particles are the main types of particulate matter and the number detected is over90%.(2) During the China Military Parade,a non-heating period with strict atmospheric control policies implemented,the spherical carbon-rich particles,which were mainly from daily activities of citizens,had the highest number abundance among all particles.(3) During normal non-heating days,abundance of vehicle-emitted soot aggregates was the highest,which showed the largest contribution of traffic to particle pollution.(4) Abundance of spherical carbon-rich particles was highest during heat-period,while the abundance of S-rich particles was significantly increased,implying the main contribution of coal combustion emission to air pollution. Combined with 48-h analysis of air mass back trajectories in 3 typical periods of atmosphere pollution,it was concluded that the local sources were themain cause of pollutants during periods with low level air pollution,while external and local sources both play an important role during periods with severe air pollution in Laishui County.
引文
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[24]牟莹莹,楼晟荣,陈长虹,等.利用SPAMS研究上海秋季气溶胶污染过程中颗粒物的老化与混合状态[J].环境科学,2013,34(6):2071-2080.MU Yingying,LOU Shengrong,CHEN Changhong,et al.Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer(SPAMS)[J].Environmental Science,2013,34(6):2071-2080.
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[26]邵龙义,时宗波.北京西北城区与清洁对照点夏季大气PMl0的微观特征及粒度分布[J].环境科学,2003,24(5):11-16.SHAO Longyi,SHI Zongbo.Microscopic characteristics and size distribution of summer PM10in the air of a northwestern urban site and a clean air site in Beijing[J].Environmental Science,2003,24(5):11-16.
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[28]李金香,董树屏,虞统,等.北京夏季典型天气TSP组成和来源对比[J].环境科学研究,2007,20(6):87-93.LI Jinxiang,DONG Shuping,YU Tong,et al.The composition and sources of TSP of Beijing in synoptic processes in summer season[J].Research of Environmental Sciences,2007,20(6):87-93.
[29]戴春岭,齐堃,康苏花,等.石家庄市大气PM10单颗粒形貌成分分析与来源识别[J].河北工业科技,2015,32(5):451-457.DAI Chunling,QI Kun,KANG Suhua,et al.Analysis of individual aerosol particle morphology and source of PM10in the air in Shijiazhuang City[J].Hebei Journal of Industrial Science and Technology,2015,32(5):451-457.
[30]李泽熙,邵龙义,樊景森,等.北京市不同天气条件下单颗粒形貌及元素组成特征[J].中国环境科学,2013,33(9):1546-1552.LI Zexi,SHAO Longyi,FAN Jingsen,et al.Morphologies and elemental compositions of individual particles under different weather conditions in Beijing[J].China Environmental Science,2013,33(9):1546-1552.
[31]赵恒,王体健,江飞,等.利用后向轨迹模式研究TRACE-P期间香港大气污染物的来源[J].热带气象学报,2009,25(2):181-186.ZHAO Heng,WANG Tijian,JIANG Fei,et al.Investigation into the source of air pollutants to Hong Kong by using backward trajectory method during the TRACE-P campaign[J].Journal of Tropical Meteorology,2009,25(2):181-186.
[32]青宪,冯桂贤,杨艳艳,等.基于后向轨迹对城市大气中二英长距离迁移来源的探讨[J].环境科学学报,2013,33(11):2959-2964.QING Xian,FENG Guixian,YANG Yanyan,et al.Long-range transport source of dioxin in the urban atmosphere based on backward trajectories[J].Acta Scientiae Circumstantiae,2013,33(11):2959-2964.
[2]王跃思,姚利,刘子锐,等.京津冀大气霾污染及控制策略思考[J].中国科学院院刊,2013(3):353-363.WANG Yuesi,YAO Li,LIU Zirui,et al.Formation of haze pollution in Beijing-Tianjin-Hebei Region and their control strategies[J].Bulletin of Chinese Academy of Science,2013(3):353-363.
[3]LI Weijun,SHAO Longyi,ZHANG Daizhou,et al.A review of single aerosol particle studies in the atmosphere of East Asia:morphology,mixing state,source and heterogeneous reactions[J].Journal of Cleaner Production,2015,112:1330-1349.
[4]GENG H,HWANG H,LIU X,et al.Investigation of aged aerosols in size-resolved Asian dust storm particles transported from Beijing,China,to Incheon,Korea,using low-Z particle EPMA[J].Atmospheric Chemistry and Physics,2014,14:3307-3323.
[5]董树屏,刘涛,孙大勇,等.用扫描电镜技术识别广州市大气颗粒物主要种类[J].岩矿测试,2001,20(3):202-207.DONG Shuping,LIU Tao,SUN Dayong,et al.Identification of major particle classes in Guangzhou aerosol by scanning electron microscopy[J].Rock and Mineral Analysis,2001,20(3):202-207.
[6]陈航宇,王京刚,董树屏,等.北京夏冬季雾霾天气大气单颗粒物特征[J].环境工程学报,2016,10(9):5023-5029.CHEN Hangyu,WANG Jinggang,DONG Shuping,et al.Character of individual aerosol particles under haze days in summer and winter in Beijing,China[J].Chinese Journal of Environmental Engineering,2016,10(9):5023-5029.
[7]HU Jun,DUAN Fengkui,HE Kebin,et al.Characteristics and mixing state of S-rich particles in haze episodes in Beijing[J].Frontiers of Environmental Science&Engineering,2016,10(5):1-10.
[8]GENG H,RYU J Y,MASKEY S,et al.Characterisation of individual aerosol particles collected during a haze episode in Incheon,Korea using the quantitative ED-EPMA technique[J].Atmospheric Chemistry and Physics,2011,11(3):1327-1337.
[9]CONG Zhiyuan,KANG Shichang,DONG Shuping,et al.Elemental and individual particle analysis of atmospheric aerosols from high Himalayas[J].Environmental Monitoring and Assessment,2010,160:323-335.
[10]LIU Xiande,ZHU Jia,VAN ESPEN P,et al.Single particle characterization of spring and summer aerosols in Beijing:formation of composite sulfate of calcium and potassium[J].Atmospheric Environment,2005,39(36):6909-6918.
[11]CONG Zhiyuan,KANG Shichang,DONG Shuping,et al.Individual particle analysis of atmospheric aerosols at Nam Co,Tibetan Plateau[J].Aerosol and Air Quality Research,2009,9:323-331.
[12]SRIVASTAVA A,JAIN V,SRIVASTAVA A.SEM-EDX analysis of various sizes aerosols in Delhi India[J].Environmental Monitoring&Assessment,2009,150(1/2/3/4):405-416.
[13]HU Tafeng,CAO Junji,HO Kinfai,et al.Winter and summer characteristics of airborne particles inside Emperor Qin's TerraCotta Museum,China:a study by scanning electron microscopyenergy dispersive X-ray spectrometry[J].Journal of the Air&Waste Management,2011,61(9):914-922.
[14]KANG E,PARK I,LEE Y J,et al.Characterization of atmospheric particles in Seoul,Korea using SEM-EDX[J].Journal of Nanoscience and Nanotechnology,2012,12(7):6016-6021.
[15]MARGIOTTA S,LETTINO A,SPERANZA A,et al.PM1geochemical and mineralogical characterization using SEM-EDX to identify particle origin-Agri Valley pilot area(Basilicata,southern Italy)[J].Natural Hazards and Earth System Sciences,2015,15(7):1551-1561.
[16]SUN Y,ZHUANG G,TANG A A,et al.Chemical characteristics of PM2.5and PM10in haze-fog episodes in Beijing[J].Environmental Science&Technology,2006,40:3148-3155.
[17]LIU Xiande,VAN ESPEN P,ADAMS F,et al.Biomass burning in southern Africa:individual particle characterization of atmospheric aerosols and savanna fire samples[J].Journal of Atmospheric Chemistry,2000,36:135-155.
[18]LI Yuwu,LIU Xiande,DONG Shuping,et al.Investigation on the geometric and matrix effects and quantitative determination of K,Cl and S atomic fraction for biomass burning particles by Monte Carlo simulation[J].Analytica Chimica Acta,2002,459(1):93-106.
[19]刘咸德,董树屏,李冰,等.沙尘暴事件中大气颗粒物化学组分的浓度变化和硫酸盐的形成[J].环境科学研究,2005,18(6):12-17.LIU Xiande,DONG Shuping,LI Bing,et al.Concentration variation of atmospheric aerosol constituents and sulfate formation during an Asian dust event[J].Research of Environmental Sciences,2005,18(6):12-17.
[20]OKYAY G,HRIPRE,REISS T,et al.Soot aggregate complex morphology:3D geometry reconstruction by SEM tomography applied on soot issued from propane combustion[J].Journal of Aerosol Science,2016,93:63-79.
[21]MORI I,NISHIKAWA M,IWASAKA Y.Chemical reaction during the coagulation of ammonium sulphate and mineral particles in the atmosphere[J].Science of the Total Environment,1998,224(1/2/3):87-91.
[22]RAM K,TRIPATHI S N,SARIN M M,et al.Primary and secondary aerosols from an urban site(Kanpur)in the Indo-Gangetic Plain:impact on CCN,CN concentrations and optical properties[J].Atmospheric Environment,2014,89:655-663.
[23]RYU S Y,KWON B G,KIM Y J,et al.Characteristics of biomass burning aerosol and its impact on regional air quality in the summer of 2003 at Gwangju,Korea[J].Atmospheric Research,2007,84:362-373.
[24]牟莹莹,楼晟荣,陈长虹,等.利用SPAMS研究上海秋季气溶胶污染过程中颗粒物的老化与混合状态[J].环境科学,2013,34(6):2071-2080.MU Yingying,LOU Shengrong,CHEN Changhong,et al.Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer(SPAMS)[J].Environmental Science,2013,34(6):2071-2080.
[25]杨书申,邵龙义.大气细颗粒物的透射电子显微镜研究[J].环境科学学报,2007,27(2):185-189.YANG Shushen,SHAO Longyi.The study of atmospheric fine particles by transmission electron microscopy[J].Acta Scientiae Circumstantiae,2007,27(2):185-189.
[26]邵龙义,时宗波.北京西北城区与清洁对照点夏季大气PMl0的微观特征及粒度分布[J].环境科学,2003,24(5):11-16.SHAO Longyi,SHI Zongbo.Microscopic characteristics and size distribution of summer PM10in the air of a northwestern urban site and a clean air site in Beijing[J].Environmental Science,2003,24(5):11-16.
[27]肖锐,刘咸德,梁汉东,等.北京市春夏季大气气溶胶的单颗粒分析表征[J].岩矿测试,2004,23(2):125-131.XIAO Rui,LIU Xiande,LIANG Handong,et al.Analytical characterization of single particle of atmospheric aerosols in spring and summer seasons in Beijing[J].Rock and Mineral Analysis,2004,23(2):125-131.
[28]李金香,董树屏,虞统,等.北京夏季典型天气TSP组成和来源对比[J].环境科学研究,2007,20(6):87-93.LI Jinxiang,DONG Shuping,YU Tong,et al.The composition and sources of TSP of Beijing in synoptic processes in summer season[J].Research of Environmental Sciences,2007,20(6):87-93.
[29]戴春岭,齐堃,康苏花,等.石家庄市大气PM10单颗粒形貌成分分析与来源识别[J].河北工业科技,2015,32(5):451-457.DAI Chunling,QI Kun,KANG Suhua,et al.Analysis of individual aerosol particle morphology and source of PM10in the air in Shijiazhuang City[J].Hebei Journal of Industrial Science and Technology,2015,32(5):451-457.
[30]李泽熙,邵龙义,樊景森,等.北京市不同天气条件下单颗粒形貌及元素组成特征[J].中国环境科学,2013,33(9):1546-1552.LI Zexi,SHAO Longyi,FAN Jingsen,et al.Morphologies and elemental compositions of individual particles under different weather conditions in Beijing[J].China Environmental Science,2013,33(9):1546-1552.
[31]赵恒,王体健,江飞,等.利用后向轨迹模式研究TRACE-P期间香港大气污染物的来源[J].热带气象学报,2009,25(2):181-186.ZHAO Heng,WANG Tijian,JIANG Fei,et al.Investigation into the source of air pollutants to Hong Kong by using backward trajectory method during the TRACE-P campaign[J].Journal of Tropical Meteorology,2009,25(2):181-186.
[32]青宪,冯桂贤,杨艳艳,等.基于后向轨迹对城市大气中二英长距离迁移来源的探讨[J].环境科学学报,2013,33(11):2959-2964.QING Xian,FENG Guixian,YANG Yanyan,et al.Long-range transport source of dioxin in the urban atmosphere based on backward trajectories[J].Acta Scientiae Circumstantiae,2013,33(11):2959-2964.
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