天津夏季边界层低层大气中PAN和O_3的输送特征分析
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摘要
采用在线仪器监测分析2017年夏季天津气象铁塔220 m观测平台大气中过氧乙酰硝酸酯(PAN)和O_3的体积分数,并结合气象观测资料和后向轨迹分析PAN和O_3的输送特征.观测期间PAN和O_3体积分数平均值分别为(0.73±0.56)×10~(-9)和(53±25)×10~(-9),最大小时体积分数分别为3.49×10~(-9)和137×10~(-9),PAN和O_3体积分数具有相似的日变化特征,白昼PAN和O_3浓度高于夜间,且PAN和O_3浓度相关系数(R2=0.52)显著高于夜间(R2=0.21).观测期间偏南风下PAN和O_3浓度最高,偏东风下最低,风玫瑰图和后向轨迹聚类分析都表明,来源于西南方向的气流轨迹对应的污染物浓度最高,途经渤海和河北、辽宁沿海地区的偏东气流对应的PAN和O_3体积分数最低,边界层内输送对PAN和O_3的体积分数分布起到了重要作用.
The volume concentration of peroxyacetyl nitrate(PAN) and O_3 in the atmosphere were measured at the Tianjin Meteorological Tower in summer 2017 by using the online instrument with meteorological parameters and back trajectory analysis to analyze the delivery characteristics of PAN and O_3.The average volume concentrations of PAN and O_3 during the observational period are(0.73 ± 0.56)×10~(-9) and(53 ± 25)×10~(-9),respectively.The hourly maximum concentrations of PAN and O_3 are 3.49×10~(-9) and 137×10~(-9).The volume concentrations of PAN and O_3 show pronounced diurnal profiles,which are both characterized by much higher values at daytime than at nighttime.In addition,the correlation coefficient between PAN and O_3 at daytime(R2=0.52) is notably higher than that at nighttime(R2=0.21).The air masses originating from the south show the highest volume concentration of PAN and O_3,with the lowest volume concentration originating from the east.The wind rose plot and cluster analysis of the back trajectories show that the highest concentration of pollutants mainly originates in the southwest.The air massess originating from the east and circulating through the Bohai Sea and coastal areas of the Hebei and Liaoning provinces show the lowest volume concentrations of PAN and O_3.The transportation within the boundary layer plays an important role in the concentration distribution of PAN and O_3.
The volume concentration of peroxyacetyl nitrate(PAN) and O_3 in the atmosphere were measured at the Tianjin Meteorological Tower in summer 2017 by using the online instrument with meteorological parameters and back trajectory analysis to analyze the delivery characteristics of PAN and O_3.The average volume concentrations of PAN and O_3 during the observational period are(0.73 ± 0.56)×10~(-9) and(53 ± 25)×10~(-9),respectively.The hourly maximum concentrations of PAN and O_3 are 3.49×10~(-9) and 137×10~(-9).The volume concentrations of PAN and O_3 show pronounced diurnal profiles,which are both characterized by much higher values at daytime than at nighttime.In addition,the correlation coefficient between PAN and O_3 at daytime(R2=0.52) is notably higher than that at nighttime(R2=0.21).The air masses originating from the south show the highest volume concentration of PAN and O_3,with the lowest volume concentration originating from the east.The wind rose plot and cluster analysis of the back trajectories show that the highest concentration of pollutants mainly originates in the southwest.The air massess originating from the east and circulating through the Bohai Sea and coastal areas of the Hebei and Liaoning provinces show the lowest volume concentrations of PAN and O_3.The transportation within the boundary layer plays an important role in the concentration distribution of PAN and O_3.
引文
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[15]Zhang J M,Wang T,Ding A J,et al.Continuous measurement of peroxyacetyl nitrate(PAN)in suburban and remote areas of western China[J].Atmospheric Environment,2009,43(2):228-237.
[16]Zhang J B,Xu Z,Yang G,et al.Peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in urban and suburban atmospheres of Beijing,China[J].Atmospheric Chemistry and Physics Discussion,2011,11(3):8173-8206.
[17]Zhang H L,Xu X B,Lin W L,et al.Wintertime peroxyacetyl nitrate(PAN)in the megacity Beijing:role of photochemical and meteorological processes[J].Journal of Environmental Sciences,2014,26(1):83-96.
[18]Wang B G,Zhu D,Zou Y,et al.Source analysis of peroxyacetyl nitrate(PAN)in Guangzhou,China:a yearlong observation study[J].Atmospheric Chemistry and Physics Discussion,2015,15(12):17093-17133.
[19]Wang B,Shao M,Roberts J M,et al.Ground-based on-line measurements of peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in the Pearl River Delta,China[J].International Journal of Environmental Analytical Chemistry,2010,90(7):548-559.
[20]Zhang G,Mu Y J,Zhou L X,et al.Summertime distributions of peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in Beijing:understanding the sources and major sink of PAN[J].Atmospheric Environment,2015,103:289-296.
[21]黄志,高天宇,赵西萌,等.2006-2014年北京夏季大气中PANs浓度变化趋势[J].北京大学学报(自然科学版),2016,52(3):528-534.Huang Z,Gao T Y,Zhao X M,et al.Trends of summertime ground-level peroxyacyl nitrates concentrations in Beijing,China from 2006 to 2014[J].Acta Scientiarum Naturalium Universitatis Pekinensis,2016,52(3):528-534.
[22]Gao T Y,Han L,Wang B,et al.Peroxyacetyl nitrate observed in Beijing in August from 2005 to 2009[J].Journal of Environmental Sciences,2014,26(10):2007-2017.
[23]Tao J C,Zhao C S,Ma N,et al.The impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2photolysis rate coefficient[J].Atmospheric Chemistry and Physics,2014,14(22):12055-12067.
[24]Kondo Y,Morino Y,Fukuda M,et al.Formation and transport of oxidized reactive nitrogen,ozone,and secondary organic aerosol in Tokyo[J].Journal of Geophysical Research,2008,113(D21):D21310,doi:10.1029/2008JD010134.
[25]Ma Z Q,Xu J,Quan W J,et al.Significant increase of surface ozone at a rural site,north of eastern China[J].Atmospheric Chemistry and Physics,2016,16(6):3969-3977.
[26]黄鹤,姚青,张文煜,等.天津夏季低层大气O3和NO2浓度垂直观测研究[J].环境科学研究,2009,22(3):315-320.Huang H,Yao Q,Zhang W Y,et al.Preliminary analysis of boundary layer O3and NO2observed in summer in Tianjin area[J].Research of Environmental Sciences,2009,22(3):315-320.
[27]贾诗卉,徐晓斌,林伟立,等.华北平原夜间对流天气对地面O3混合比抬升效应[J].应用气象学报,2015,26(3):280-290.Jia S H,Xu X B,Lin W L,et al.Increased mixing ratio of surface ozone by nighttime convection process over the North China Plain[J].Journal of Applied Meteorological Science,2015,26(3):280-290.
[28]马志强,王跃思,孙扬,等.北京大气中常规污染物的垂直分布特征[J].环境科学研究,2007,20(5):1-6.Ma Z Q,Wang Y S,Sun Y,et al.Characteristics of vertical air pollutants in Beijing[J].Research of Environmental Sciences,2007,20(5):1-6.
[29]姚青,孙玫玲,蔡子颖,等.2009年天津城区地面O3和NOX的季节变化与相关性分析[J].环境化学,2011,30(9):1650-1656.Yao Q,Sun M L,Cai Z Y,et al.Seasonal variation and analysis of the relationship between NO,NO2and O3concentrations in Tianjin in 2009[J].Environmental Chemistry,2011,30(9):1650-1656.
[30]杨俊益,辛金元,吉东生,等.2008~2011年夏季京津冀区域背景大气污染变化分析[J].环境科学,2012,33(11):3693-3704.Yang J Y,Xin J Y,Ji D S,et al.Variation analysis of background atmospheric pollutants in North China during the summer of 2008 to 2011[J].Environmental Science,2012,33(11):3693-3704.
[31]Hartsell B E,Aneja V P,Lonneman W A.Relationships between peroxyacetyl nitrate,O3,and NOyat the rural Southern Oxidants Study site in central Piedmont,North Carolina,site SONIA[J].Journal of Geophysical Research,1994,99(D10):21033-21041.
[32]范洋,樊曙先,张红亮,等.临安冬夏季SO2、NO2和O3体积分数特征及与气象条件的关系[J].大气科学学报,2013,36(1):121-128.Fan Y,Fan S X,Zhang H L,et al.Characteristics of SO2,NO2,O3volume fractions and their relationship with weather conditions at Linan in summer and winter[J].Transactions of Atmospheric Sciences,2013,36(1):121-128.
[33]姚青,韩素芹,蔡子颖.天津一次持续低能见度事件的影响因素分析[J].气象,2012,38(6):688-694.Yao Q,Han S Q,Cai Z Y.Analysis of related factors for a case of low horizontal visibility in Tianjin[J].Meteorological Monthly,2012,38(6):688-694.
[2]Liu Z,Wang Y H,Gu D S,et al.Evidence of reactive aromatics as a major source of peroxy acetyl nitrate over China[J].Environmental Science&Technology,2010,44(18):7017-7022.
[3]Honrath R E,Hamlin A J,Merrill J T.Transport of ozone precursors from the Arctic troposphere to the North Atlantic region[J].Journal of Geophysical Research:Atmospheres,1996,101(D22):29335-29351.
[4]Kondo Y,Koike M,Kawakami S,et al.Profiles and partitioning of reactive nitrogen over the Pacific Ocean in winter and early spring[J].Journal of Geophysical Research:Atmospheres,1997,102(D23):28405-28424.
[5]Singh H B,Herlth D,Kolyer R,et al.Reactive nitrogen and ozone over the western Pacific:distribution,partitioning,and sources[J].Journal of Geophysical Research:Atmospheres,1996,101(D1):1793-1808.
[6]Hudman R C,Jacob D J,Cooper O R,et al.Ozone production in transpacific Asian pollution plumes and implications for ozone air quality in California[J].Journal of Geophysical Research:Atmospheres,2004,109(D23):D23S10.
[7]Mc Fadyen G G,Cape J N.Peroxyacetyl nitrate in eastern Scotland[J].Science of the Total Environment,2005,337(1-3):213-222.
[8]Kleindienst T E.Recent developments in the chemistry and biology of peroxyacetyl nitrate[J].Research on Chemical Intermediates,1994,20(3-5):335-384.
[9]Grosjean D,Woodhouse L F.Peroxyacetyl nitrate and peroxypropionyl nitrate during SCOS 97-NARSTO[J].Environmental Science&Technology,2001,35(20):4007-4014.
[10]Jiang Z,Worden J R,Payne V H,et al.Ozone export from East Asia:the role of PAN[J].Journal of Geophysical Research:Atmospheres,2016,121(11):6555-6563.
[11]张剑波,唐孝炎.大气中PAN的测定及其与前体物的关系[J].环境化学,1994,13(1):30-39.Zhang J B,Tang X Y.Atmospheric PAN measurements and the formation of PAN in various systems[J].Environmental Chemistry,1994,13(1):30-39.
[12]王斌,张剑波.夏季北京市大气中PAN与PPN的监测分析[J].环境科学,2007,28(7):1621-1626.Wang B,Zhang J B.Monitoring and analysis of PAN and PPN in the air of Beijing during the summer of 2005[J].Environmental Science,2007,28(7):1621-1626.
[13]杨光,张剑波,王斌.2006年夏季北京大气中PAN与PPN浓度变化和相关性分析[J].北京大学学报(自然科学报),2009,45(1):144-150.Yang G,Zhang J B,Wang B.Analysis on correlation and concentration variation of atmospheric PAN and PPN in Beijing[J].Acta Scientiarum Naturalium Universitatis Pekinensis,2009,45(1):144-150.
[14]韩丽,张剑波,王凤.2010年世博会期间上海大气中PAN和PPN的监测分析[J].北京大学学报(自然科学版),2013,49(3):497-503.Han L,Zhang J B,Wang F.Online measurement of PAN and PPN in Shanghai during the World Expo,2010[J].Acta Scientiarum Naturalium Universitatis Pekinensis,2013,49(3):497-503.
[15]Zhang J M,Wang T,Ding A J,et al.Continuous measurement of peroxyacetyl nitrate(PAN)in suburban and remote areas of western China[J].Atmospheric Environment,2009,43(2):228-237.
[16]Zhang J B,Xu Z,Yang G,et al.Peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in urban and suburban atmospheres of Beijing,China[J].Atmospheric Chemistry and Physics Discussion,2011,11(3):8173-8206.
[17]Zhang H L,Xu X B,Lin W L,et al.Wintertime peroxyacetyl nitrate(PAN)in the megacity Beijing:role of photochemical and meteorological processes[J].Journal of Environmental Sciences,2014,26(1):83-96.
[18]Wang B G,Zhu D,Zou Y,et al.Source analysis of peroxyacetyl nitrate(PAN)in Guangzhou,China:a yearlong observation study[J].Atmospheric Chemistry and Physics Discussion,2015,15(12):17093-17133.
[19]Wang B,Shao M,Roberts J M,et al.Ground-based on-line measurements of peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in the Pearl River Delta,China[J].International Journal of Environmental Analytical Chemistry,2010,90(7):548-559.
[20]Zhang G,Mu Y J,Zhou L X,et al.Summertime distributions of peroxyacetyl nitrate(PAN)and peroxypropionyl nitrate(PPN)in Beijing:understanding the sources and major sink of PAN[J].Atmospheric Environment,2015,103:289-296.
[21]黄志,高天宇,赵西萌,等.2006-2014年北京夏季大气中PANs浓度变化趋势[J].北京大学学报(自然科学版),2016,52(3):528-534.Huang Z,Gao T Y,Zhao X M,et al.Trends of summertime ground-level peroxyacyl nitrates concentrations in Beijing,China from 2006 to 2014[J].Acta Scientiarum Naturalium Universitatis Pekinensis,2016,52(3):528-534.
[22]Gao T Y,Han L,Wang B,et al.Peroxyacetyl nitrate observed in Beijing in August from 2005 to 2009[J].Journal of Environmental Sciences,2014,26(10):2007-2017.
[23]Tao J C,Zhao C S,Ma N,et al.The impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2photolysis rate coefficient[J].Atmospheric Chemistry and Physics,2014,14(22):12055-12067.
[24]Kondo Y,Morino Y,Fukuda M,et al.Formation and transport of oxidized reactive nitrogen,ozone,and secondary organic aerosol in Tokyo[J].Journal of Geophysical Research,2008,113(D21):D21310,doi:10.1029/2008JD010134.
[25]Ma Z Q,Xu J,Quan W J,et al.Significant increase of surface ozone at a rural site,north of eastern China[J].Atmospheric Chemistry and Physics,2016,16(6):3969-3977.
[26]黄鹤,姚青,张文煜,等.天津夏季低层大气O3和NO2浓度垂直观测研究[J].环境科学研究,2009,22(3):315-320.Huang H,Yao Q,Zhang W Y,et al.Preliminary analysis of boundary layer O3and NO2observed in summer in Tianjin area[J].Research of Environmental Sciences,2009,22(3):315-320.
[27]贾诗卉,徐晓斌,林伟立,等.华北平原夜间对流天气对地面O3混合比抬升效应[J].应用气象学报,2015,26(3):280-290.Jia S H,Xu X B,Lin W L,et al.Increased mixing ratio of surface ozone by nighttime convection process over the North China Plain[J].Journal of Applied Meteorological Science,2015,26(3):280-290.
[28]马志强,王跃思,孙扬,等.北京大气中常规污染物的垂直分布特征[J].环境科学研究,2007,20(5):1-6.Ma Z Q,Wang Y S,Sun Y,et al.Characteristics of vertical air pollutants in Beijing[J].Research of Environmental Sciences,2007,20(5):1-6.
[29]姚青,孙玫玲,蔡子颖,等.2009年天津城区地面O3和NOX的季节变化与相关性分析[J].环境化学,2011,30(9):1650-1656.Yao Q,Sun M L,Cai Z Y,et al.Seasonal variation and analysis of the relationship between NO,NO2and O3concentrations in Tianjin in 2009[J].Environmental Chemistry,2011,30(9):1650-1656.
[30]杨俊益,辛金元,吉东生,等.2008~2011年夏季京津冀区域背景大气污染变化分析[J].环境科学,2012,33(11):3693-3704.Yang J Y,Xin J Y,Ji D S,et al.Variation analysis of background atmospheric pollutants in North China during the summer of 2008 to 2011[J].Environmental Science,2012,33(11):3693-3704.
[31]Hartsell B E,Aneja V P,Lonneman W A.Relationships between peroxyacetyl nitrate,O3,and NOyat the rural Southern Oxidants Study site in central Piedmont,North Carolina,site SONIA[J].Journal of Geophysical Research,1994,99(D10):21033-21041.
[32]范洋,樊曙先,张红亮,等.临安冬夏季SO2、NO2和O3体积分数特征及与气象条件的关系[J].大气科学学报,2013,36(1):121-128.Fan Y,Fan S X,Zhang H L,et al.Characteristics of SO2,NO2,O3volume fractions and their relationship with weather conditions at Linan in summer and winter[J].Transactions of Atmospheric Sciences,2013,36(1):121-128.
[33]姚青,韩素芹,蔡子颖.天津一次持续低能见度事件的影响因素分析[J].气象,2012,38(6):688-694.Yao Q,Han S Q,Cai Z Y.Analysis of related factors for a case of low horizontal visibility in Tianjin[J].Meteorological Monthly,2012,38(6):688-694.
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