武汉市大气VOCs污染特征及其对臭氧生成的影响
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摘要
于2014年1-12月在武汉市城区对大气中105种挥发性有机化合物(VOCs)进行在线监测,以便研究武汉市区VOCs的组成特征及变化规律。同时评估大气VOCs对武汉市臭氧(O_3)生成的影响,并探讨关键VOCs活性物种及来源。结果表明,武汉市2014年大气总挥发性有机化合物(TVOCs)年平均浓度为(92.88±1.06)μg/cm~3,乙烷、丙烷、乙烯、正丁烷、甲苯是浓度最大的5个物种。大气TVOCs的浓度在冬季最高夏季最低,昼夜变化表现为明显的早晚双高峰特征。在非甲烷碳氢化合物(NMHCs)中,烯炔烃的臭氧生成潜势最大,其次为芳香烃和烷烃。武汉市臭氧生成潜势最大的5个物种分别为乙烯、间/对-二甲苯、丙烯、甲苯和异丁烯。机动车排放是武汉市大气VOCs的重要来源,控制机动车VOCs排放有助于削减大气VOCs活性较大的组分,从而减少臭氧的生成。
Ambient volatile organic compounds(VOCs)were continuously measured from January 2014 to December 2014at an urban site in Wuhan.The characteristics of VOCs and their effect on ozone formation were studied.The total VOCs(TVOCs)concentration was(92.88±1.06)μg/cm~3,and among all VOCs,ethane,propane,ethene,n-butane,benzene,toluene,i-butane,ethyne,i-pentane and m/p-xylene were the most abundant species.TVOCs was the highest in winter and the lowest in summer.The concentrations of TVOCs showed a small peak in the morning,then decreased to their minimums in the afternoon,and reached steadily high levels at night.Ethene,m/p-xylene,propene,i-butene and toluene were the main contributors to ozone production,and vehicle exhaust was an important source of VOCs in Wuhan.Controlling vehicle related VOCs will reduce ozone production in Wuhan.
Ambient volatile organic compounds(VOCs)were continuously measured from January 2014 to December 2014at an urban site in Wuhan.The characteristics of VOCs and their effect on ozone formation were studied.The total VOCs(TVOCs)concentration was(92.88±1.06)μg/cm~3,and among all VOCs,ethane,propane,ethene,n-butane,benzene,toluene,i-butane,ethyne,i-pentane and m/p-xylene were the most abundant species.TVOCs was the highest in winter and the lowest in summer.The concentrations of TVOCs showed a small peak in the morning,then decreased to their minimums in the afternoon,and reached steadily high levels at night.Ethene,m/p-xylene,propene,i-butene and toluene were the main contributors to ozone production,and vehicle exhaust was an important source of VOCs in Wuhan.Controlling vehicle related VOCs will reduce ozone production in Wuhan.
引文
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[30]Barletta B,Meinardi S,Rowland F S,et al.Volatile organic compounds in 43 Chinese cities[J].Atmospheric Environment,2005,39(32):5979-5990.
[31]Chang C,Wang J,Lung S C,et al.Source characterization of ozone precursors by complementary approaches of vehicular indicator and principal component analysis[J].Atmospheric Environment,2009,43(10):1771-1778.
[2]Li J,Lu K,Lyu W,et al.Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006-2011[J].Journal of Environmental Sciences,2014,26(1):23-36.
[3]Xue L K,Wang T,Gao J,et al.Ground-level ozone in four Chinese cities:precursors,regional transport and heterogeneous processes[J].Atmospheric Chemistry and Physics,2014,14(23):13175-13188.
[4]Ling Z H,Guo H,Cheng H R,et al.Sources of ambient volatile organic compounds and their contributions to photochemical ozone formation at a site in the Pearl River Delta,southern China[J].Environmental Pollution,2011,159(10):2310-2319.
[5]Ding A J,Fu C B,Yang X Q,et al.Ozone and fine particle in the western Yangtze River Delta:an overview of 1 yr data at the SORPES station[J].Atmospheric Chemistry and Physics,2013,13(11):5813-5830.
[6]Tie X,Geng F,Guenther A,et al.Megacity impacts on regional ozone formation:observations and WRF-Chem modeling for the MIRAGE-Shanghai field campaign[J].Atmospheric Chemistry and Physics,2013,13(11):5655-5669.
[7]Li G H,Cheng S Y,Li J B,et al.Characterization of ambient ozone and its precursors around a coking plant[J].Environmental Monitoring and Assessment,2014,186(5):3165-3179.
[8]Cheng H,Guo H,Wang X,et al.On the relationship between ozone and its precursors in the Pearl River Delta:application of an observation-based model(OBM)[J].Environmental Science and Pollution Research,2010,17(3):547-560.
[9]Wang J L,Wang C H,Lai C H,et al.Characterization of ozone precursors in the Pearl River Delta by time series observation of non-methane hydrocarbons[J].Atmospheric Environment,2008,42(25):6233-6246.
[10]Zhang J,Wang T,Chameides W L,et al.Source characteristics of volatile organic compounds during high ozone episodes in Hong Kong,Southern China[J].Atmospheric Chemistry and Physics,2008,8(16):4983-4996.
[11]Guo H,Wang T,Simpson I J,et al.Source contributions to ambient VOCs and CO at a rural site in Eastern China[J].Atmospheric Environment,2004,38(27):4551-4560.
[12]陆思华,白郁华,张广山,等.大气中挥发性有机化合物(VOCs)的人为来源研究[J].环境科学学报,2006(5):757-763.Lu Sihua,Bai Yuhua,Zhang Guangshan,et al.Source apportionment of anthropogenic emissions of volatile organic compounds[J].Acta Scientiae Circumstantiae,2006(5):757-763.
[13]Ou J M,Zheng J Y,Li R R,et al.Speciated OVOC and VOC emission inventories and their implications for reactivity:based ozone control strategy in the Pearl River Delta region,China[J].Science of the Total Environment,2015(530):393-402.
[14]Ling Z H,Guo H.Contribution of VOC sources to photochemical ozone formation and its control policy implication in Hong Kong[J].Environmental Science&Policy,2014(38):180-191.
[15]陈宜然,陈长虹,王红丽,等.上海臭氧及前体物变化特征与相关性研究[J].中国环境监测,2011(5):44-49.Chen Yiran,Chen Changhong,Wang Hongli,et al.Analysis on concentration variety characteristics of ozone and correlations with its precursors in Shanghai[J].Environmental Monitoring in China,2011(5):44-49.
[16]陆玉霞,邵平,安俊琳.南京北郊夏季大气光化学污染特征研究[J].环境科学与技术,2015,38(3):102-107.Lu Yuxia,Shao Ping,An Junlin,et al.Characteristics of atmospheric photochemical pollution during summer in Nanjing northern suburb[J].Environmental Science&Technology,2015,38(3):102-107.
[17]Song Y,Dai W,Shao M,et al.Comparison of receptor models for source apportionment of volatile organic compounds in Beijing,China[J].Environmental Pollution,2008,156(1):174-183.
[18]罗玮,王伯光,刘舒乐,等.广州大气挥发性有机物的臭氧生成潜势及来源研究[J].环境科学与技术,2011,34(5):80-86.Luo Wei,Wang Boguang,Liu Shule,et al.VOC ozone formation potential and emission sources in the atmosphere of Guangzhou[J].Environmental Sciences&Technology,2011,34(5):80-86.
[19]Cai C,Geng F,Tie X,et al.Characteristics and source apportionment of VOCs measured in Shanghai,China[J].Atmospheric Environment,2010,44(38):5005-5014.
[20]Jia C H,Mao X X,Huang T,et al.Non-methane hydrocarbons(NMHCs)and their contribution to ozone formation potential in a petrochemical industrialized city,northwest China[J].Atmospheric Research,2016(169):225-236.
[21]Atkinson R,Arey J.Atmospheric degradation of volatile organic compounds[J].Chemical Reviews,2003,103(12):4605-4638.
[22]Carter W P L.Development of ozone reactivity scales for volatile organic compounds[J].Journal of the Air&Waste Management Association,1994,44(7):881-899.
[23]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.
[24]Guo H,So K L,Simpson I J,et al.C1–C8volatile organic compounds in the atmosphere of Hong Kong:overview of atmospheric processing and source apportionment[J].Atmospheric Environment,2007,41(7):1456-1472.
[25]Zhang J,Wang Y,Wu F,et al.Nonmethane hydrocarbon measurements at a suburban site in Changsha City,China[J].Science of the Total Environment,2009,408(2):312-317.
[26]Lyu X P,Chen N,Guo H,et al.Ambient volatile organic compounds and their effect on ozone production in Wuhan,central China[J].Science of the Total Environment,2016(541):200-209.
[27]Liu Y,Shao M,Fu L,et al.Source profiles of volatile organic compounds(VOCs)measured in China:Part I[J].Atmospheric Environment,2008,42(25):6247-6260.
[28]Christensen C S,Skov H,Palmgren F.C5–C8non-methane hydrocarbon measurements in Copenhagen:concentrations,sources and emission estimates[J].Science of the Total Environment,1999,236(1/2/3):163-171.
[29]Zhang Y L,Wang X M,Zhang Z,et al.Sources of C2-C4alkenes,the most important ozone nonmethane hydrocarbon precursors in the Pearl River Delta region[J].Science of the Total Environment,2015(502):236-245.
[30]Barletta B,Meinardi S,Rowland F S,et al.Volatile organic compounds in 43 Chinese cities[J].Atmospheric Environment,2005,39(32):5979-5990.
[31]Chang C,Wang J,Lung S C,et al.Source characterization of ozone precursors by complementary approaches of vehicular indicator and principal component analysis[J].Atmospheric Environment,2009,43(10):1771-1778.