长沙市大气中醛酮类化合物浓度变化特征
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摘要
参照美国环保署EPA-TO11标准方法,于2014年7—10月监测了长沙市大气中醛酮类化合物的质量浓度。主要监测到的醛酮类化合物为甲醛、乙醛、丙酮、丙醛、甲基丙烯醛,夏季质量浓度最高的是甲醛(13. 86 mg/m~3),其次是乙醛(7. 28 mg/m~3)、丙酮(7. 14 mg/m~3),秋季质量浓度最高的是甲醛(10. 31 mg/m~3),其次是丙酮(8. 37 mg/m~3)、乙醛(5. 78 mg/m~3)。夏季醛酮类化合物的总量高于秋季,甲醛、乙醛、丙酮的质量浓度最大值基本出现在13:00—15:00。C1/C2(甲醛/乙醛)、C2/C3(乙醛/丙醛)的平均值分别为2. 02、10. 19。分析了醛酮类化合物之间的相关性以及它们可能的来源。丙醛和甲醛、乙醛的相关性较好,三者有共同的人为来源。夏季大气中除丙酮外,其他醛酮类化合物的相关性均较好。夏季甲基丙烯醛和甲醛、乙醛、丙酮有相同的自然来源。综合分析可知,长沙大气中醛酮类化合物质量浓度受自然因素和人为因素的双重影响。
The levels of carbonyl compounds in ambient air of Changsha City were measured from July 2014 to October 2014,referred to EPA-T011 method. Formaldehyde,acetaldehyde,acetone,propionaldehyde and MACR( methacrolein) were the predominant carbonyls in Changsha city. The highest concentration was formaldehyde( 13. 86 mg/m~3),followed by acetaldehyde( 7. 28 mg/m~3) and acetone( 7. 14 mg/m~3) in summer,and the highest concentration was formaldehyde( 10. 31 mg/m~3),followed by acetone( 8. 37 mg/m~3) and acetaldehyde( 5. 78 mg/m~3) in autumn. The total amount of carbonyls in summer was higher than that in autumn,and the maximum concentrations of formaldehyde,acetaldehyde,and acetone mostly appeared at 13: 00-15: 00.The average values of C1/C2( formaldehyde/acetaldehyde) and C2/C3( acetaldehyde/propionaldehyde) were 2. 02 and 10. 19,respectively. The correlation between carbonyls and their possible sources were analyzed. The correlation between propionaldehyde and formaldehyde and acetaldehyde was good,and they had the same human sources. The correlation of carbonyls in the atmosphere was good in summer except acetone. In summer,methacrolein and acetaldehyde,acetone had the same natural source. In summary,the concentration of carbonyls in the ambient air in Changsha were affected by both natural and human factors.
The levels of carbonyl compounds in ambient air of Changsha City were measured from July 2014 to October 2014,referred to EPA-T011 method. Formaldehyde,acetaldehyde,acetone,propionaldehyde and MACR( methacrolein) were the predominant carbonyls in Changsha city. The highest concentration was formaldehyde( 13. 86 mg/m~3),followed by acetaldehyde( 7. 28 mg/m~3) and acetone( 7. 14 mg/m~3) in summer,and the highest concentration was formaldehyde( 10. 31 mg/m~3),followed by acetone( 8. 37 mg/m~3) and acetaldehyde( 5. 78 mg/m~3) in autumn. The total amount of carbonyls in summer was higher than that in autumn,and the maximum concentrations of formaldehyde,acetaldehyde,and acetone mostly appeared at 13: 00-15: 00.The average values of C1/C2( formaldehyde/acetaldehyde) and C2/C3( acetaldehyde/propionaldehyde) were 2. 02 and 10. 19,respectively. The correlation between carbonyls and their possible sources were analyzed. The correlation between propionaldehyde and formaldehyde and acetaldehyde was good,and they had the same human sources. The correlation of carbonyls in the atmosphere was good in summer except acetone. In summer,methacrolein and acetaldehyde,acetone had the same natural source. In summary,the concentration of carbonyls in the ambient air in Changsha were affected by both natural and human factors.
引文
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[23]王芳,冯艳丽,姜知明,等.上海大气中气相和颗粒相羰基化合物研究[J].科技导报,2015,33(6):13-19.WANG Fang,FENG Yanli,JIANG Zhiming,et al.Gaseous and Particulate Carbonyl Compounds in Shanghai Ambient Air[J].Science&Technology Review,2015,33(6):13-19.
[24]CERóN-BRETóN J G,CERóN-BRETóN R M.Carbonyls in the Urban Atmosphere of Monterrey,Mexico:Sources,Exposure,and Health Risk[J].Air Quality Atmosphere and Health,2017,10:53-67.
[25]DUTTA C,SOM D,CHATTERJEE A,et al.Mixing Ratios of Carbonyls and BTEX in Ambient Air of Kolkata,India and Their Associated Health Risk[J].Environmental Monitoring Assessment,2009,148:97-107.
[2]POSSANZINI M,PALO V D,PRETICCA M,et al.Measurements of Lower Carbonyls in Rome Ambient Air[J].Atmospheric Environment,1996,30(22):3 757-3 764.
[3]LUI K H,et al.Seasonal Behavior of Carbonyls and Source Characterization of Formaldehyde(HCHO)in Ambient Air[J].Atmosphere Environment,2017,152:51-60.
[4]ALTSHULLER A P.Assessment of the Contribution of Chemical Species to the Eye Irritation Potential of Photochemical Smog[J].Atmospheric Chemistry,1978,(28):594-598.
[5]OCHS S M,ALBUQUERQUE F C,et al.Evaluation of C1-C13 Carbonyl Compounds by RRLC-UV in the Atmosphere of Niterói City,Brazil[J].Atmospheric Environment,2011,45(29):5 183-5 190.
[6]JIANG Z H,GROSSELIN B,DA?LE V,MELLOUKIA,MU Y J.Seasonal,Diurnal and Nocturnal Variations of Carbonyl Compounds in the Semi-Urban Environment of Orléans,France[J].Environmental Sciences,2016,40:84-91.
[7]魏恩棋,时庭锐,尹彦勋,等.天津市大气中羰基化合物特征[J].中国环境监测,2011,27(2):37-41.WEI Enqi,Shi Tingrui,Yin Yanxun,et al.The Pollution Characterizations of Carbonyls in the Atmosphere of Tianjin[J].Environmental Monitoring in China,2011,27(2):37-41.
[8]吕辉雄,文晟,盛国英,等.广州市灰霾与非灰霾期间大气中的低分子量羰基化合物[J].环境化学,2009,28(4):562-566.LYU Huixiong,WEN Sheng,SHENG Guoying,et al.Low-Molecular-Weight Carbonyl Compounds in Ambient Air During Haze and Non-haze Periods in Guangzhou,China[J].Environmental Chemistry,2009,28(4):562-566.
[9]LYU H X,WEN S,SHENG G Y,FU J M.Seasonal and Diurnal Variations of Carbonyl Compounds in the Urban Atmosphere of Guangzhou,China[J].Science Total Environment,2010,408(17):3 523-3 529.
[10]姜荻.沈阳市环境空气中醛酮类化合物污染现状初探[J].环境保护科学,2015,41(3):118-119,158.JIANG Di.Current Pollution Status of Aldoketones Compounds in the Ambient Air of Shenyang[J].Environmental Protection Science,2015,41(3):118-119,158.
[11]USEPA,Compendium of Methods for the Determination of Toxic Organic Compounds in Ambient Air[R].Washington DC:Center for Environmental Research Information Office of Research and Development USEnvironmental Protection Agency,1996.
[12]ATKINSON R.Atmospheric Chemistry of VOCs and NOx[J].Atmospheric Environment,2000,34(12-14):2 063-2 101.
[13]LOUIS J S,HANWANT B S.Measurements of Formaldehyde and Acetaldehyde in the Urban Ambient Air[J].Atmospheric Environment,1986,20(6):1 301-1 304.
[14]HO K F,Lee S C.Seasonal Variation of Carbonyl Compound Concentrations in Urban Area of Hong Kong[J].Atmosphere Environment,2002,36:1 259-1 265.
[15]VILLANUEVA I,POPP C J,MARTIN R S.Biogenic Emissions and Ambient Concentrations of Hydrocarbons,Carbonyl Compounds and Organic Acids from Ponderosa Pine and Cottonwood Trees at Rural and Forested Sites in Central New Mexico[J].Atmospheric Environment,2004,38(2):249-260.
[16]JACOB D J,WOFSY S C.Photochemistry of Biogenic Emissions over the Amazon Forest[J].Journal of Geographical Research,1988,93:1 477-1 486.
[17]ANDERSON L G,LANNING J A,BARRELL R,et al.Sources and Sinks of Formaldehyde and Acetaldehyde:An Analysis of Denver's Ambient Concentration Data[J].Atmospheric Environment,1996,30(12):2 113-2 123.
[18]JI Y M,GAO Y P,LI G Y,et al.Theoretical Study of the Reaction Mechanism and Kinetics of LowMolecular-Weight Atmospheric Aldehydes(C1-C4)with NO2[J].Atmosphere Environment,2012,54:288-295.
[19]徐竹,庞小兵,牟玉静.北京市大气和降雨中醛酮化合物的污染研究[J].环境科学学报,2006,26(12):1 948-1 954.XU Zhu,PANG Xiaobing,MU Yujing.Measurement of Carbonyl Compounds in Beijing Ambient Air and Rain[J].Acta Scientiae Circumstantiae,2006,26(12):1 948-1 954.
[20]GUO S J,CHEN M,TAN J H.Seasonal and Diurnal Characteristics of Atmospheric Carbonyls in Nanning,China[J].Atmospheric Research,2016,169:46-53.
[21]CHENG Y,LEE S C,HUANG Y,et al.Diurnal and Seasonal Trends of Carbonyl Compounds in Roadside,Urban,and Suburban Environment of Hong Kong[J].Atmospheric Environment,2014,89:43-51.
[22]蒋朝晖,王玉娇,郑玄,等.张家界森林大气中醛酮类化合物浓度变化特征[J].环境科学研究,2016,29(9):1 272-1 278.JIANG Zhaohui,WANG Yujiao,ZHENG Xuan,et al.Variation Characteristics of Atmospheric Carbonyl Compounds in Zhangjiajie Forest[J].Research of Environment Sciences,2016,29(9):1 272-1 278.
[23]王芳,冯艳丽,姜知明,等.上海大气中气相和颗粒相羰基化合物研究[J].科技导报,2015,33(6):13-19.WANG Fang,FENG Yanli,JIANG Zhiming,et al.Gaseous and Particulate Carbonyl Compounds in Shanghai Ambient Air[J].Science&Technology Review,2015,33(6):13-19.
[24]CERóN-BRETóN J G,CERóN-BRETóN R M.Carbonyls in the Urban Atmosphere of Monterrey,Mexico:Sources,Exposure,and Health Risk[J].Air Quality Atmosphere and Health,2017,10:53-67.
[25]DUTTA C,SOM D,CHATTERJEE A,et al.Mixing Ratios of Carbonyls and BTEX in Ambient Air of Kolkata,India and Their Associated Health Risk[J].Environmental Monitoring Assessment,2009,148:97-107.