万州城区空气污染过程中含碳气溶胶的变化特征
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摘要
于2016年9月28日至10月15日在万州城区对气态污染物、颗粒物及其含碳气溶胶进行了在线连续观测,结合气象参数,分析了含碳气溶胶的污染特征。结果表明,此次持续污染过程主要由颗粒物污染造成,污染天PM_(10)和PM_(2.5)平均质量浓度分别为170.8、123.7μg/m~3,显著高于非污染天。污染天和非污染天PM_(2.5)、NO_x、有机碳(OC)及元素碳(EC)浓度的日变化都呈双峰,但污染天PM_(2.5)、NO_x和OC出现早峰值时间比非污染天推迟1～3h。污染天OC、EC的平均质量浓度分别为28.0、5.4μg/m~3,分别为非污染天的2.2、1.6倍。以非污染天的起始点作为参照点,得到污染天OC、EC的平均增长率分别为159.3%和73.0%,OC污染累积和二次转化贡献率分别为45.8%和54.2%,说明污染过程OC以二次转化为主。并用最小比值法估算了二次有机碳(SOC)含量,得到污染天和非污染天PM_(2.5)中SOC平均质量浓度分别为16.3、5.3μg/m~3,SOC在OC中的占比(以质量分数计)分别为56.1%和39.9%,污染天SOC占比增加,也证明污染过程OC以二次转化为主。污染天静风出现频率比非污染天高,在东南风的影响下,OC、EC易出现高浓度。
Continuous measurements of gas pollutants,particulates and carbonaceous aerosols contained were conducted to assess the characteristics of carbonaceous aerosols during a typical air pollution event in the urban Wanzhou from September 28th to October 15th,2016.The results showed that,this continuous pollution process was mainly caused by particulate pollution.The average concentrations of PM_(10) and PM_(2.5) during polluted days were 170.8 and 123.7μg/m~3,respectively,higher than those during non-polluted days.The diurnal variations of PM_(2.5),NO_x,organic carbon(OC)and elemental carbon(EC)showed significantly bimodal pattern in both polluted days and nonpolluted days.However,the morning peak times of PM_(2.5),NO_x,and OC concentrations were delayed by about one to three hours during the polluted days.The average OC and EC concentrations were 28.0 and 5.4μg/m~3 during polluted days,which were 2.2 and 1.6 times of non-polluted days,respectively.Compared to the reference point(the first day of non-polluted day),the average growth rates of OC and EC were 159.3% and 73.0% during polluted days.It was estimated the secondary formation was more important than the accumulation process for the increase of OC during polluted days,which accounting for 54.2% and 45.8%,respectively.The secondary organic carbon(SOC)concentrations were estimated by the minimum OC/EC,and the concentrations of SOC during polluted days and nonpolluted days were 16.3 and 5.3μg/m~3,accounting for 56.1% and 39.9% to OC,respectively,also verifying the secondary formation source.Higher static wind ratio appeared during polluted days and OC and EC concentrations were generally higher under southeastern conditions.
Continuous measurements of gas pollutants,particulates and carbonaceous aerosols contained were conducted to assess the characteristics of carbonaceous aerosols during a typical air pollution event in the urban Wanzhou from September 28th to October 15th,2016.The results showed that,this continuous pollution process was mainly caused by particulate pollution.The average concentrations of PM_(10) and PM_(2.5) during polluted days were 170.8 and 123.7μg/m~3,respectively,higher than those during non-polluted days.The diurnal variations of PM_(2.5),NO_x,organic carbon(OC)and elemental carbon(EC)showed significantly bimodal pattern in both polluted days and nonpolluted days.However,the morning peak times of PM_(2.5),NO_x,and OC concentrations were delayed by about one to three hours during the polluted days.The average OC and EC concentrations were 28.0 and 5.4μg/m~3 during polluted days,which were 2.2 and 1.6 times of non-polluted days,respectively.Compared to the reference point(the first day of non-polluted day),the average growth rates of OC and EC were 159.3% and 73.0% during polluted days.It was estimated the secondary formation was more important than the accumulation process for the increase of OC during polluted days,which accounting for 54.2% and 45.8%,respectively.The secondary organic carbon(SOC)concentrations were estimated by the minimum OC/EC,and the concentrations of SOC during polluted days and nonpolluted days were 16.3 and 5.3μg/m~3,accounting for 56.1% and 39.9% to OC,respectively,also verifying the secondary formation source.Higher static wind ratio appeared during polluted days and OC and EC concentrations were generally higher under southeastern conditions.
引文
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[3]CAO J J,LEE S C,HO K F,et al.Spatial and seasonal variations of atmospheric organic carbon and elemental carbon in Pearl River Delta Region,China[J].Atmospheric Environment,2004,38(27):4447-4456.
[4]BATMUNKH T,KIM Y J,LEE K Y,et al.Time-resolved measurements of PM2.5carbonaceous aerosols at Gosan,Korea[J].Journal of the Air&Waste Management Association,2014,61(11):1174-1182.
[5]MOORE K F,NING Z,NTZIACHRISTOS L,et al.Daily variation in the properties of urban ultrafine aerosol-Part I:physical characterization and volatility[J].Atmospheric Environment,2007,41(38):8633-8646.
[6]ALVES,PIO C A,CASIMIRO A.Secondary organic compounds in atmospheric aerosols:speciation and formation mechanisms[J].Journal of the Brazilian Chemical Society,2005,16(5):1017-1029.
[7]谢绍东,于淼,姜明.有机气溶胶的来源与形成研究现状[J].环境科学学报,2006,26(12):1933-1939.
[8]于建华,虞统,杨晓光,等.北京冬季PM2.5中元素碳、有机碳的污染特征[J].环境科学研究,2004,17(1):48-50.
[9]PATHAK R K,WANG T,HO K F,et al.Characteristics of summertime PM2.5organic and elemental carbon in four major Chinese cities:implications of high acidity for water-soluble organic carbon(WSOC)[J].Atmospheric Environment,2011,45(2):318-325.
[10]JACOBSON M Z.Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols[J].Nature,2001,409(6821):695-697.
[11]ZHANG R J,CAO J J,LEE S C,et al.Carbonaceous aerosols in PM10and pollution gases in winter in Beijing[J].Journal of Environmental Sciences,2007,19(5):564-571.
[12]MAUDERLY J L,CHOW J C.Health effects of organic aerosols[J].Inhalation Toxicology,2008,20(3):257-288.
[13]HAND J L,SCHICHTEL B A,MALM W C,et al.Spatial and temporal trends in PM2.5organic and elemental carbon across the United States[J].Advances in Meteorology,2013,2013:367674.
[14]PARASKEVOPOULOU D,LIAKAKOU E,GERASOPOU-LOS E,et al.Long-term characterization of organic and elemental carbon in the PM2.5 fraction:the case of Athens,Greece[J].Atmospheric Chemistry and Physics,2014,14(23):13313-13325.
[15]LIN P,HU M,DENG Z,et al.Seasonal and diurnal variations of organic carbon in PM2.5in Beijing and the estimation of secondary organic carbon[J].Journal of Geophysical Research,2009,114(D2):1-14.
[16]FENG Y L,CHEN Y J,GUO H,et al.Characteristics of organic and elemental carbon in PM2.5 samples in Shanghai,China[J].Atmospheric Research,2009,92(4):434-442.
[17]CAO J J,WU F,CHOW J C,et al.Characterization and source apportionment of atmospheric organic and elemental carbon during fall and winter of 2003in Xi’an,China[J].Atmospheric Chemistry and Physics,2005,5(11):3127-3137.
[18]YANG F,TAN J,ZHAO Q,et al.Characteristics of PM2.5speciation in representative megacities and across China[J].Atmospheric Chemistry and Physics,2011,11(11):5207-5219.
[19]陈刚才,陶俊,赵琦,等.重庆主城区大气总悬浮颗粒中有机碳和元素碳污染特征分析[J].重庆环境科学,2003,25(10):1-4.
[20]李礼,余家燕.重庆城区空气中有机碳和元素碳浓度水平的监测分析[J].重庆环境科学,2012,34(2):41-43.
[21]张灿,周志恩,翟崇治,等.基于重庆本地碳成分谱的PM2.5碳组分来源分析[J].环境科学,2014,35(3):810-819.
[22]赵亮,鲁群岷,李莉,等.重庆万州区大气降水的化学特征[J].重庆环境科学,2013,35(2):9-15.
[23]彭超,翟崇治,王欢博,等.万州城区夏季、冬季PM2.5中有机碳和元素碳的浓度特征[J].环境科学学报,2015,35(6):1638-1644.
[24]周敏,陈长虹,王红丽,等.上海秋季典型大气高污染过程中有机碳和元素碳的变化特征[J].环境科学学报,2013,33(1).
[25]云龙龙,陆钒,张天舒,等.无锡市冬季典型天气PM2.5中碳组分的污染特征[J].环境科学,2014,35(9):3280-3286.
[26]APPEL B R,COLODNY P.Analysis of carbonaceous materials in Southern California atmospheric aerosols[J].Environmental Science&Techology,1976,10(4):359-363.
[27]CHOW J C,WATSON J G,LU Z,et al.Descriptive analysis of PM2.5and PM10at regionally representative locations during SJVAQS/AUSPEX[J].Atmosperic Environment,1996,30(12):2079-2112.
[28]CASTRO L M,PIO C A,HARRISON R M,et al.Carbonaceous aerosol in urban and rural European atmospheres:estimation of secondary organic carbon concentrations[J].Atmosperic Environment,1999,33(17):2771-2781.
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