济南市背景区域大气PM_(2.5)污染特征及其对能见度的影响
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摘要
为研究背景地区大气PM_(2. 5)化学组分季节变化特征及对能见度的影响,本研究于2016年春、夏、秋、冬在济南市七星台采集大气PM_(2. 5)样品,分析其中水溶性离子组分及OC、EC的污染特征并研究其区域传输贡献.结果表明,NH_4~+、SO_4~(2-)和NO_3~-三者之和占年均离子总浓度的90. 24%,二次生成的水溶性无机离子污染较为严重. NO_3~-/SO_4~(2-)呈现出明显的冬高夏低的季节性变化特征.各季节的SO_4~(2-)和NH_4~+主要以(NH4)2SO4结合的形式存在. SOC/OC的范围是21. 17%～54. 21%,表明该地区存在较为严重的二次有机污染.四季SOR值均大于0. 1,显示本区域四季均有SO_4~(2-)的二次生成,四季NOR的值均高于SOR,可知NO2的二次转化强于SO2的二次转化.大气消光系数(Bext)的范围是172. 68～320. 61 Mm-1,年均值为256. 48Mm-1,大气消光系数呈现明显的夏低冬高的季节性趋势.后推气流轨迹显示七星台地区春、夏季主要受长距离传输和海洋源的影响,秋、冬季主要受局地源的影响.对比2008年济南市大气PM_(2. 5)污染特征研究,结果显示机动车对大气环境影响显著提升.
In order to study the seasonal variations in the chemical composition of atmospheric particulate matter with diameters less than 2. 5 μm( PM_(2. 5)) and its influence on visibility in background areas,atmospheric PM_(2. 5) samples were collected in spring,summer,autumn,and winter 2016 at Qixingtai in Ji'nan. The pollution characteristics of water-soluble ions components,organic carbon( OC),and elemental carbon( EC) were analyzed,and their regional transmission contributions were studied. The results show that NH_4~+,SO_4~(2-),and NO_3~-were the main components of water-soluble ions,accounting for 90. 24% of the annual total ion concentration. The secondary water soluble inorganic ions were polluted severely. NO_3~-/SO_4~(2-)presented obvious seasonal variations of high( low) levels in winter( summer). In each season,SO_4~(2-)and NH_4~+existed mainly in the form of( NH4)2 SO4. The value of secondary OC( SOC)/OC ranged from 21. 17% to 54. 21%,indicating the presence of relatively severe secondary organic pollution in this area. The sulfur oxidation ratio( SOR) value in all seasons was greater than 0. 1,indicating that the secondary generation of SO_4~(2-)occurs in all seasons in this region,and the value of nitrogen oxidation ratio( NOR) in all seasons was higher than the SOR value. The secondary transformation of NO2 in the Qixingtai region was stronger than that of SO2. The range of atmospheric extinction coefficient( Bext) was 172. 68-320. 61 Mm-1,with an annual mean of 256. 48 Mm-1. The atmospheric extinction coefficient showed an obvious seasonal trend of the lowest( highest) in summer( winter). The backward airflow trajectory shows that the Qixingtai was affected mainly by the long-distance transmission from Northwest China and the ocean in spring and summer and by local sources in autumn and winter. A comparison of the characteristics of atmospheric PM_(2. 5) pollution in Ji'nan in 2008 revealed that the influence of motor vehicles on the atmospheric environment has been significantly improved.
In order to study the seasonal variations in the chemical composition of atmospheric particulate matter with diameters less than 2. 5 μm( PM_(2. 5)) and its influence on visibility in background areas,atmospheric PM_(2. 5) samples were collected in spring,summer,autumn,and winter 2016 at Qixingtai in Ji'nan. The pollution characteristics of water-soluble ions components,organic carbon( OC),and elemental carbon( EC) were analyzed,and their regional transmission contributions were studied. The results show that NH_4~+,SO_4~(2-),and NO_3~-were the main components of water-soluble ions,accounting for 90. 24% of the annual total ion concentration. The secondary water soluble inorganic ions were polluted severely. NO_3~-/SO_4~(2-)presented obvious seasonal variations of high( low) levels in winter( summer). In each season,SO_4~(2-)and NH_4~+existed mainly in the form of( NH4)2 SO4. The value of secondary OC( SOC)/OC ranged from 21. 17% to 54. 21%,indicating the presence of relatively severe secondary organic pollution in this area. The sulfur oxidation ratio( SOR) value in all seasons was greater than 0. 1,indicating that the secondary generation of SO_4~(2-)occurs in all seasons in this region,and the value of nitrogen oxidation ratio( NOR) in all seasons was higher than the SOR value. The secondary transformation of NO2 in the Qixingtai region was stronger than that of SO2. The range of atmospheric extinction coefficient( Bext) was 172. 68-320. 61 Mm-1,with an annual mean of 256. 48 Mm-1. The atmospheric extinction coefficient showed an obvious seasonal trend of the lowest( highest) in summer( winter). The backward airflow trajectory shows that the Qixingtai was affected mainly by the long-distance transmission from Northwest China and the ocean in spring and summer and by local sources in autumn and winter. A comparison of the characteristics of atmospheric PM_(2. 5) pollution in Ji'nan in 2008 revealed that the influence of motor vehicles on the atmospheric environment has been significantly improved.
引文
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[17]张秋晨,朱彬,龚佃利.南京地区大气气溶胶及水溶性无机离子特征分析[J].中国环境科学,2014,34(2):311-316.Zhang Q C,Zhu B,Gong D L. Characterization of water-soluble ion species of aerosol in Nanjing, China[J]. China Environmental Science,2014,34(2):311-316.
[18]姚青,韩素芹,毕晓辉.天津2009年3月气溶胶化学组成及其消光特性研究[J].中国环境科学,2012,32(2):214-220.Yao Q, Han S Q, Bi X H, et al. Main components and extinction characteristic of aerosol during March 2009 at Tianjin[J]. China Environmental Science,2012,32(2):214-220.
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[20] Wang Y,Zhuang G S,Zhang X Y,et al. The ion chemistry,seasonal cycle,and sources of PM2. 5and TSP aerosol in Shanghai[J]. Atmospheric Environment,2006,40(16):2935-2952.
[21] Chow J C,Watson J G,Lu Z Q,et al. Descriptive analysis of PM2. 5and PM10at regionally representative locations during SJVAQS/AUSPEX[J]. Atmospheric Environment,1996,30(12):2079-2112.
[22]吴丹,蔺少龙,杨焕强,等.杭州市PM2. 5中水溶性离子的污染特征及其消光贡献[J].环境科学,2017,38(7):2656-2666.Wu D,Lin S L,Yang H Q,et al. Pollution characteristics and light extinction contribution of water-soluble ions of PM2. 5in Hangzhou[J]. Environmental Science,2017,38(7):2656-2666.
[23]汤莉莉,沈宏雷,汤蕾,等.冬季南京北郊大气气溶胶中水溶性阴离子特征[J].大气科学学报,2013,36(4):489-498.Tang L L,Shen H L,Tang L,et al. Characteristics of watersoluble anions in atmospheric aerosol in northern suburb of Nanjing in winter[J]. Transactions of Atmospheric Sciences,2013,36(4):489-498.
[24]沙丹丹,王红磊,朱彬,等.冬季PM2. 5中含碳气溶胶的污染特征———长江三角洲地区一次区域重污染过程分析[J].中国环境科学,2017,37(10):3611-3622.Sha D D,Wang H L,Zhu B,et al. Pollution characteristics of carbonaceous aerosols in PM2. 5during a regional heavy air pollution episode in winter in the Yangtze River Delta[J]. China Environmental Science,2017,37(10):3611-3622.
[25] Turpin B J,Cary R A,Huntzicker J J. An in situ,time-resolved analyzer for aerosol organic and elemental carbon[J]. Aerosol Science and Technology,1990,12(1):161-171.
[26] Turpin B J,Huntzicker J J. Identification of secondary organic aerosol episodes and quantitation of primary and secondary organic aerosol concentrations during SCAQS[J]. Atmospheric Environment,1995,29(23):3527-3544.
[27]刘晓迪,孟静静,侯战方,等.济南市夏、冬季PM2. 5中化学组分的季节变化特征及来源解析[J].环境科学,2018,39(9):4014-4025.Liu X D,Meng J J,Hou Z F,et al. Analysis of seasonal variations in chemical characteristics and sources of PM2. 5during summer and winter in Ji'nan City[J]. Environmental Science,2018,39(9):4014-4025.
[28] Pitchford M,Malm W,Schichtel B. et al. 2007. Revised algorithm for estimating light extinction from IMPROVE particle speciation data[J]. Journal of the Air&Waste Management Association,2007,57(11):1326-1336.
[29]徐昶,叶辉,沈建东,等.杭州大气颗粒物散射消光特性及霾天气污染特征[J].环境科学,2014,35(12):4422-4430.Xu C, Ye H, She J D, et al. Light scattering extinction properties of atmospheric particle and pollution characteristics in hazy weather in Hangzhou[J]. Environmental Science,2014,35(12):4422-4430.
[30]谭学士.天津市大气颗粒物中OC/EC污染特征与细粒径来源解析[D].北京:北京化工大学,2015.Tan X S. Concentration and size distribution of OC/EC in atmospheric aerosol in Tianjin,China[D]. Beijing:Beijing University of Chemical Technology,2015.
[31]向洪,余家燕,王军,等.重庆城区能见度特征与颗粒物消光贡献[J].环境科学与技术,2018,41(7):110-116.Xiang H, Yu J Y, Wang J, et al. Study on visibility characteristics of Chongqing's urban area and the extinction contribution by particulate matter[J]. Environmental Science and Technology,2018,41(7):110-116.
[2]杨复沫,贺克斌,马永亮,等.北京PM2. 5浓度的变化特征及其与PM10、TSP的关系[J].中国环境科学,2002,22(6):506-510.Yang F M,He K B,Ma Y L,et al. Variation characteristics of PM2. 5concentration and its relationship with PM10 and TSP in Beijing[J]. China Environmental Science,2002,22(6):506-510.
[3] Zhang T,Cao J J,Tie X X,et al. Water-soluble ions in atmospheric aerosols measured in Xi'an, China:seasonal variations and sources[J]. Atmospheric Research,2011,102(1-2):110-119.
[4]康晖,朱彬,王红磊,等.长三角典型站点冬季大气PM2. 5中OC、EC污染特征[J].环境科学,2018,39(3):961-971.Kang H,Zhu B,Wang H L,et al. Characterization and variation of organic carbon(OC)and elemental carbon(EC)in PM2. 5during the winter in the Yangtze River delta region,China[J].Environmental Science,2018,39(3):961-971.
[5]赵亚南,王跃思,温天雪,等.长白山PM2. 5中水溶性无机离子观测研究[J].环境化学,2011,30(4):812-815.Zhao Y N,Wang Y S,Wen T X,et al. Observation and analysis of water-soluble inorganic ions in PM2. 5from mount Changbai[J]. Environmental Chemistry,2011,30(4):812-815.
[6]杨雨蒙,杨凌霄,张俊美,等.济南市冬季灰霾日PM1. 0和PM1. 0-2. 5污染特征[J].山东大学学报(工学版),2017,47(2):111-116.Yang Y M,Yang L X,Zhang J M,et al. Characteristics of PM1. 0and PM1. 0-2. 5in haze days during winter in Jinan[J].Journal of Shandong University(Engineering Science),2017,47(2):111-116.
[7] Gao X M,Yang L X,Cheng S H,et al. Semi-continuous measurement of water-soluble ions in PM2. 5in Jinan,China:temporal variations and source apportionments[J]. Atmospheric Environment,2011,45(33):6048-6056.
[8]陶月乐,李亲凯,张俊,等.成都市大气颗粒物粒径分布及水溶性离子组成的季节变化特征[J].环境科学,2017,38(10):4034-4043.Tao Y L,Li Q K,Zhang J,et al. Seasonal variations in particle size distribution and water-soluble ion composition of atmospheric particles in Chengdu[J]. Environmental Science,2017,38(10):4034-4043.
[9]韩月梅,沈振兴,曹军骥,等.西安市大气颗粒物中水溶性无机离子的季节变化特征[J].环境化学,2009,28(2):261-266.Han Y M,Shen Z X,Cao J J,et al. Seasonal variations of water-soluble inorganic ions in atmospheric particles over Xi'an[J]. Environmental Chemistry,2009,28(2):261-266.
[10]王璐,温天雪,苗红妍,等.太原大气颗粒物中水溶性无机离子质量浓度及粒径分布特征[J].环境科学,2016,37(9):3249-3257.Wang L,Wen T X,Miao H Y,et al. Concentrations and size distributions of water-soluble inorganic ions in aerosol particles in Taiyuan,Shanxi[J]. Environmental Science,2016,37(9):3249-3257.
[11]赵亚南,王跃思,温天雪,等.贡嘎山大气气溶胶中水溶性无机离子的观测与分析研究[J].环境科学,2009,30(1):9-13.Zhao Y N,Wang Y S,Wen T X,et al. Observation and analysis on water-soluble inorganic chemical compositions of atmospheric aerosol in Gongga Mountain[J]. Environmental Science,2009,30(1):9-13.
[12] Meng Z Y,Seinfeld J H. On the source of the submicrometer droplet mode of urban and regional aerosols[J]. Aerosol Science and Technology,1994,20(3):253-265.
[13] Lee Y L, Sequeira R. Water-soluble aerosol and visibility degradation in Hong Kong during autumn and early winter,1998[J]. Environmental Pollution,2002,116(2):225-233.
[14]徐昶.中国特大城市气溶胶的理化特性、来源及其形成机制[D].上海:复旦大学,2010.Xu C. Characteristics,source and the formation mechanism of aerosol in mega-city,China[D]. Shanghai:Fudan University,2010.
[15]杨凌霄.济南市大气PM2. 5污染特征、来源解析及其对能见度的影响[D].济南:山东大学,2008.Yang L X. Characteristics,source apportionment and influence on visual range of PM2. 5in Jinan[D]. Jinan:Shandong University,2008.
[16]姬洪亮,赵宏,孔少飞,等.天津近岸海域大气颗粒物无机组分季节变化及源析[J].中国环境科学,2011,31(2):177-185.Ji H L,Zhao H,Kong S F,et al. Seasonal variation of inorganic composition in ambient particulate matter in Tianjin offshore area and its source analysis[J]. China Environmental Science,2011,31(2):177-185.
[17]张秋晨,朱彬,龚佃利.南京地区大气气溶胶及水溶性无机离子特征分析[J].中国环境科学,2014,34(2):311-316.Zhang Q C,Zhu B,Gong D L. Characterization of water-soluble ion species of aerosol in Nanjing, China[J]. China Environmental Science,2014,34(2):311-316.
[18]姚青,韩素芹,毕晓辉.天津2009年3月气溶胶化学组成及其消光特性研究[J].中国环境科学,2012,32(2):214-220.Yao Q, Han S Q, Bi X H, et al. Main components and extinction characteristic of aerosol during March 2009 at Tianjin[J]. China Environmental Science,2012,32(2):214-220.
[19] Wang Y,Zhang G S,Tang A H,et al. The ion chemistry and the source of PM2. 5aerosol in Beijing[J]. Atmospheric Environment,2005,39(21):3771-3784.
[20] Wang Y,Zhuang G S,Zhang X Y,et al. The ion chemistry,seasonal cycle,and sources of PM2. 5and TSP aerosol in Shanghai[J]. Atmospheric Environment,2006,40(16):2935-2952.
[21] Chow J C,Watson J G,Lu Z Q,et al. Descriptive analysis of PM2. 5and PM10at regionally representative locations during SJVAQS/AUSPEX[J]. Atmospheric Environment,1996,30(12):2079-2112.
[22]吴丹,蔺少龙,杨焕强,等.杭州市PM2. 5中水溶性离子的污染特征及其消光贡献[J].环境科学,2017,38(7):2656-2666.Wu D,Lin S L,Yang H Q,et al. Pollution characteristics and light extinction contribution of water-soluble ions of PM2. 5in Hangzhou[J]. Environmental Science,2017,38(7):2656-2666.
[23]汤莉莉,沈宏雷,汤蕾,等.冬季南京北郊大气气溶胶中水溶性阴离子特征[J].大气科学学报,2013,36(4):489-498.Tang L L,Shen H L,Tang L,et al. Characteristics of watersoluble anions in atmospheric aerosol in northern suburb of Nanjing in winter[J]. Transactions of Atmospheric Sciences,2013,36(4):489-498.
[24]沙丹丹,王红磊,朱彬,等.冬季PM2. 5中含碳气溶胶的污染特征———长江三角洲地区一次区域重污染过程分析[J].中国环境科学,2017,37(10):3611-3622.Sha D D,Wang H L,Zhu B,et al. Pollution characteristics of carbonaceous aerosols in PM2. 5during a regional heavy air pollution episode in winter in the Yangtze River Delta[J]. China Environmental Science,2017,37(10):3611-3622.
[25] Turpin B J,Cary R A,Huntzicker J J. An in situ,time-resolved analyzer for aerosol organic and elemental carbon[J]. Aerosol Science and Technology,1990,12(1):161-171.
[26] Turpin B J,Huntzicker J J. Identification of secondary organic aerosol episodes and quantitation of primary and secondary organic aerosol concentrations during SCAQS[J]. Atmospheric Environment,1995,29(23):3527-3544.
[27]刘晓迪,孟静静,侯战方,等.济南市夏、冬季PM2. 5中化学组分的季节变化特征及来源解析[J].环境科学,2018,39(9):4014-4025.Liu X D,Meng J J,Hou Z F,et al. Analysis of seasonal variations in chemical characteristics and sources of PM2. 5during summer and winter in Ji'nan City[J]. Environmental Science,2018,39(9):4014-4025.
[28] Pitchford M,Malm W,Schichtel B. et al. 2007. Revised algorithm for estimating light extinction from IMPROVE particle speciation data[J]. Journal of the Air&Waste Management Association,2007,57(11):1326-1336.
[29]徐昶,叶辉,沈建东,等.杭州大气颗粒物散射消光特性及霾天气污染特征[J].环境科学,2014,35(12):4422-4430.Xu C, Ye H, She J D, et al. Light scattering extinction properties of atmospheric particle and pollution characteristics in hazy weather in Hangzhou[J]. Environmental Science,2014,35(12):4422-4430.
[30]谭学士.天津市大气颗粒物中OC/EC污染特征与细粒径来源解析[D].北京:北京化工大学,2015.Tan X S. Concentration and size distribution of OC/EC in atmospheric aerosol in Tianjin,China[D]. Beijing:Beijing University of Chemical Technology,2015.
[31]向洪,余家燕,王军,等.重庆城区能见度特征与颗粒物消光贡献[J].环境科学与技术,2018,41(7):110-116.Xiang H, Yu J Y, Wang J, et al. Study on visibility characteristics of Chongqing's urban area and the extinction contribution by particulate matter[J]. Environmental Science and Technology,2018,41(7):110-116.
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