广州番禺大气成分站一次典型光化学污染过程PAN和O_3分析
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摘要
通过对广州番禺大气成分站(GPACS)的光化学相关污染物(O_3、PAN、VOCs、NO_2、NO)以及气象要素进行观测,分析2010～2016年期间发生在广州地区一次典型光化学污染过程.结果表明,该光化学污染过程期间,O_3和PAN总体体积分数比较高,最大O_3小时体积分数为140. 6×10~(-9),而最大PAN小时体积分数为4. 7×10~(-9). NO整体体积分数较低,对O_3的化学滴定和PAN的去除影响较小. NO_2整体体积分数较高、辐射较强和风速较低则有利于O_3和PAN的形成和积累. PAN和O_3具有一定的线性关系(R~2=0. 55),而形成PAN和O_3前体物VOCs物种不完全相同影响着它们的线性关系,在生成PAN的VOCs物种中,乙烯、丙烷、异戊二烯和甲苯所占的比例较大,而对臭氧生成潜势较大的物种有异戊二烯、1,3,5-三甲苯、丙烯、间,对-二甲苯以及甲苯.对PA自由基体积分数进行估算,发现它的日均值体积分数在0. 11×10~(-12)～0. 16×10~(-12)范围变化,远高于其它地区,表明此次发生的光化学反应较为强烈.
The typical photochemical pollution process in Guangzhou was analyzed from 2010 to 2016 by observing photochemical pollutants( ozone( O_3),peroxyacetyl nitrate( PAN),volatile organic compounds( VOCs),nitrogen dioxide( NO_2),and nitric oxide( NO)) and meteorological factors at the Guangzhou Panyu Atmospheric Composition Station( GPACS). The results showed that during this photochemical pollution process,the average O_3 and PAN concentrations were relatively high: O_3,max1 h concentration was 140. 6× 10~(-9) and PANmax1 h concentration was 4. 7 × 10~(-9). The average concentration of NO was low,which had little effect on O_3 titration and PAN elimination. The high NO_2 concentration,strong radiation,and low wind speed all led to the formulation and accumulation of O_3 and PAN. The linear relationship between O_3 and PAN( R~2= 0. 55) was affected by the fact that their precursor VOCs were not similar. Ethene,propane,isoprene,and toluene had a large influence in PAN formation,while isoprene,1,3,5-trimethylbenzene,propene,m,p-xylene,and toluene had a large influence on O_3 formation potential. When evaluating PA concentration,we found that its daily average concentration ranged from 0. 11 × 10~(-12) to 0. 16 × 10~(-12),which were higher than many places around the world,indicating that this photochemical process was relatively intensive.
The typical photochemical pollution process in Guangzhou was analyzed from 2010 to 2016 by observing photochemical pollutants( ozone( O_3),peroxyacetyl nitrate( PAN),volatile organic compounds( VOCs),nitrogen dioxide( NO_2),and nitric oxide( NO)) and meteorological factors at the Guangzhou Panyu Atmospheric Composition Station( GPACS). The results showed that during this photochemical pollution process,the average O_3 and PAN concentrations were relatively high: O_3,max1 h concentration was 140. 6× 10~(-9) and PANmax1 h concentration was 4. 7 × 10~(-9). The average concentration of NO was low,which had little effect on O_3 titration and PAN elimination. The high NO_2 concentration,strong radiation,and low wind speed all led to the formulation and accumulation of O_3 and PAN. The linear relationship between O_3 and PAN( R~2= 0. 55) was affected by the fact that their precursor VOCs were not similar. Ethene,propane,isoprene,and toluene had a large influence in PAN formation,while isoprene,1,3,5-trimethylbenzene,propene,m,p-xylene,and toluene had a large influence on O_3 formation potential. When evaluating PA concentration,we found that its daily average concentration ranged from 0. 11 × 10~(-12) to 0. 16 × 10~(-12),which were higher than many places around the world,indicating that this photochemical process was relatively intensive.
引文
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[17]周炎,岳玎利,钟流举,等.广东鹤山地区夏季大气中PAN污染特征[J].环境监测管理与技术,2013,25(4):24-27.Zhou Y,Yue D L,Zhong L J,et al. Properties of atmospheric PAN pollution in Heshan during summer time[J]. The Administration and Technique of Environmental Monitoring,2013,25(4):24-27.
[18]邹宇,邓雪娇,李菲,等.广州番禺大气成分站复合污染过程VOCs对O3与SOA的生成潜势[J].环境科学,2017,38(6):2246-2255.Zou Y,Deng X J,Li F,et al. Effect of VOCs on O3and SOA formation potential during the combined pollution process in Guangzhou Panyu atmospheric composition station[J].Environmental Science,2017,38(6):2246-2255.
[19]邹宇,邓雪娇,王伯光,等.广州番禺大气成分站挥发性有机物的污染特征[J].中国环境科学,2013,33(5):808-813.Zou Y,Deng X J,Wang B G,et al. Pollution characteristics of volatile organic compounds in Panyu composition station[J].China Environmental Science,2013,33(5):808-813.
[20]邹宇,邓雪娇,李菲,等.广州大气中异戊二烯浓度变化特征、化学活性和来源分析[J].环境科学学报,2015,35(3):647-655.Zou Y, Deng X J, Li F, et al. Variation characteristics,chemical reactivity and sources of isoprene in the atmosphere of Guangzhou[J]. Acta Scientiae Circumstantiae,2015,35(3):647-655.
[21] Dunlea E J,Herndon S C,Nelson D D,et al. Evaluation of nitrogen dioxide chemiluminescence monitors in a polluted urban environment[J]. Atmospheric Chemistry and Physics,2007,7(10):2691-2704.
[22] Li Y,Lau A K H,Fung J C H,et al. Importance of NOxcontrol for peak ozone reduction in the Pearl River Delta region[J].Journal of Geophysic Research,2013,118(16):9428-9443.
[23] 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.
[24] Zheng J Y,Zhang L J,Che W W,et al. A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta region,China and its uncertainty assessment[J].Atmospheric Environment,2009,43(32):5112-5122.
[25]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(自然科学版),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.
[26] 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.
[27] Lee G, Jang Y, Lee H, et al. Characteristic behavior of peroxyacetyl nitrate(PAN)in Seoul Megacity, Korea[J].Chemosphere,2008,73(4):619-628.
[28] Hartsell B E, Aneja V P, Lonneman W A. Relationships between peroxyacetyl nitrate,O3,and NOy at the rural Southern Oxidants Study site in central Piedmont,North Carolina,site SONIA[J]. Journal of Geophysic Research,1994,99(D10):21033-21041.
[29] Atkinson R,Baulch D L,Cox R A,et al. Evaluated kinetic,photochemical and heterogeneous data for atmospheric chemistry:supplement V. IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry[J]. Journal of Physical and Chemical Reference Data,1997,26(3):521-1011.
[30] Demore W B,Sander S P,Golden D M,et al. Chemical kinetics and photochemical data for use in stratospheric modeling[D].Pasadena,CA:Jet Propulsion Laboratory,California Institute of Technology,1997. 1-266.
[31] Aneja V P,Hartsell B E,Kim D S,et al. Peroxyacetyl nitrate in Atlanta,Georgia:Comparison and analysis of ambient data for suburban and downtown locations[J]. Journal of the Air&Waste Management Association,1999,49(2):177-184.
[32] 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.
[2] Zou Y,Deng X J,Zhu D,et al. Characteristics of 1 year of observational data of VOCs,NOxand O3at a suburban site in Guangzhou,China[J]. Atmospheric Chemistry and Physics,2015,15(12):6625-6636.
[3] Wang T,Wei X L,Ding A J,et al. Increasing surface ozone concentrations in the background atmosphere of Southern China,1994-2007[J]. Atmospheric Chemistry and Physics,2009,9(16):6217-6227.
[4] 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.
[5] La Franchi B W,Wolfe G M,Thornton J A,et al. Closing the peroxy acetyl nitrate budget:observations of acyl peroxy nitrates(PAN, PPN, and MPAN)during BEARPEX 2007[J].Atmospheric Chemistry and Physics,2009,9(19):7623-7641.
[6]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.
[7] Nielsen T,Samuelsson U,Grennfelt P,et al. Peroxyacetyl nitrate in long-range transported polluted air[J]. Nature,1981,293(5833):553-555.
[8]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.
[9] Zhang G,Mu Y J,Liu J F,et al. Seasonal and diurnal variations of atmospheric peroxyacetyl nitrate, peroxypropionyl nitrate,and carbon tetrachloride in Beijing[J]. Journal of Environmental Sciences,2014,26(1):65-74.
[10] Lee Y C,Shindell D T,Faluvegi G,et al. Increase of ozone concentrations,its temperature sensitivity and the precursor factor in South China[J]. Tellus B:Chemical and Physical Meteorology,2014,66(1):23455.
[11] Ran L,Zhao C S,Xu W Y,et al. VOC reactivity and its effect on ozone production during the Ha Chi summer campaign[J].Atmospheric Chemistry and Physics,2011,11(10):4657-4667.
[12]陆克定,张远航,苏杭,等.珠江三角洲夏季臭氧区域污染及其控制因素分析[J].中国科学:化学,2010,40(4):407-420.Lu K D,Zhang Y H,Su H,et al. Regional ozone pollution and key controlling factors of photochemical ozone production in Pearl River Delta during summer time[J]. Scientia Sinica Chimica,2010,40(4):407-420.
[13]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.
[14] 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.
[15]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.
[16] 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.
[17]周炎,岳玎利,钟流举,等.广东鹤山地区夏季大气中PAN污染特征[J].环境监测管理与技术,2013,25(4):24-27.Zhou Y,Yue D L,Zhong L J,et al. Properties of atmospheric PAN pollution in Heshan during summer time[J]. The Administration and Technique of Environmental Monitoring,2013,25(4):24-27.
[18]邹宇,邓雪娇,李菲,等.广州番禺大气成分站复合污染过程VOCs对O3与SOA的生成潜势[J].环境科学,2017,38(6):2246-2255.Zou Y,Deng X J,Li F,et al. Effect of VOCs on O3and SOA formation potential during the combined pollution process in Guangzhou Panyu atmospheric composition station[J].Environmental Science,2017,38(6):2246-2255.
[19]邹宇,邓雪娇,王伯光,等.广州番禺大气成分站挥发性有机物的污染特征[J].中国环境科学,2013,33(5):808-813.Zou Y,Deng X J,Wang B G,et al. Pollution characteristics of volatile organic compounds in Panyu composition station[J].China Environmental Science,2013,33(5):808-813.
[20]邹宇,邓雪娇,李菲,等.广州大气中异戊二烯浓度变化特征、化学活性和来源分析[J].环境科学学报,2015,35(3):647-655.Zou Y, Deng X J, Li F, et al. Variation characteristics,chemical reactivity and sources of isoprene in the atmosphere of Guangzhou[J]. Acta Scientiae Circumstantiae,2015,35(3):647-655.
[21] Dunlea E J,Herndon S C,Nelson D D,et al. Evaluation of nitrogen dioxide chemiluminescence monitors in a polluted urban environment[J]. Atmospheric Chemistry and Physics,2007,7(10):2691-2704.
[22] Li Y,Lau A K H,Fung J C H,et al. Importance of NOxcontrol for peak ozone reduction in the Pearl River Delta region[J].Journal of Geophysic Research,2013,118(16):9428-9443.
[23] 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.
[24] Zheng J Y,Zhang L J,Che W W,et al. A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta region,China and its uncertainty assessment[J].Atmospheric Environment,2009,43(32):5112-5122.
[25]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(自然科学版),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.
[26] 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.
[27] Lee G, Jang Y, Lee H, et al. Characteristic behavior of peroxyacetyl nitrate(PAN)in Seoul Megacity, Korea[J].Chemosphere,2008,73(4):619-628.
[28] Hartsell B E, Aneja V P, Lonneman W A. Relationships between peroxyacetyl nitrate,O3,and NOy at the rural Southern Oxidants Study site in central Piedmont,North Carolina,site SONIA[J]. Journal of Geophysic Research,1994,99(D10):21033-21041.
[29] Atkinson R,Baulch D L,Cox R A,et al. Evaluated kinetic,photochemical and heterogeneous data for atmospheric chemistry:supplement V. IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry[J]. Journal of Physical and Chemical Reference Data,1997,26(3):521-1011.
[30] Demore W B,Sander S P,Golden D M,et al. Chemical kinetics and photochemical data for use in stratospheric modeling[D].Pasadena,CA:Jet Propulsion Laboratory,California Institute of Technology,1997. 1-266.
[31] Aneja V P,Hartsell B E,Kim D S,et al. Peroxyacetyl nitrate in Atlanta,Georgia:Comparison and analysis of ambient data for suburban and downtown locations[J]. Journal of the Air&Waste Management Association,1999,49(2):177-184.
[32] 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.
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