宜宾市冬季挥发性有机物污染特征及来源
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摘要
为了解宜宾市冬季VOCs(volatile organic compounds,挥发性有机物)污染特征,于2016年12月选取宜宾市2个国控环境监测点位,采集冬季环境空气VOCs样品,利用三级冷阱预浓缩仪-气相色谱质谱联用仪(GC-MS)测定大气中89种VOCs物种,分析VOCs体积分数及其物种组成情况,并对其主要来源进行识别.结果表明:宜宾市区冬季环境空气中φ(VOCs)平均值为35.10×10~(-9),φ(VOCs)最高值和最低值分别为67.34×10~(-9)、20.58×10~(-9);监测VOCs物种类别中芳香烃占比最高,其次为烷烃、卤代烃;体积分数较大的VOCs物种主要为苯、甲苯、氯甲烷、二氯甲烷、异丁烷、异丙醇、正丁烷等.CMB(化学质量平衡)模型源解析宜宾市冬季环境空气VOCs的六大主要贡献源分别为移动源、油气挥发源、溶剂使用源、工艺过程源、生物质燃烧源和其他源.以2015年为基准年,利用排放因子法对宜宾市VOCs进行排放量计算发现,宜宾市VOCs年排放量为39.54×10~3t,其中,工艺过程源、溶剂使用源、移动源、化石燃料燃烧源的贡献率分别为35.5%、24.5%、28.9%、8.0%.研究显示,对宜宾市冬季环境空气中VOCs贡献率较大的污染源分别为移动源、溶剂使用源、工艺过程源等。
In order to understand the characteristics of volatile organic compounds in Yibin City in winter,air samples were collected at two sites in December 2016.Eighty-nine species of volatile organic compounds(VOCs)were measured by using pre-concentration-GC-MS method.This study investigated the volume fraction of VOCs and its ingredients.In addition,the main sources of VOCs were also identified.The results showed that the average volume fraction of VOCs was 35.10×10~(-9),and the highest volume fraction was 67.34×10~(-9)while the lowest volume fraction was 20.58×10~(-9).Aromatic hydrocarbons were the highest proportion in the monitored species category,followed by alkanes and halogenated hydrocarbons.Species with a large volume fraction were benzene,toluene,methyl chloride,dichloromethane,isobutene,isopropanol,n-butane and so on.Source apportionment for VOCs in Yibin City was taken by CMB model and emission inventory method.The CMB results indicated 6 major contribution sources of VOCs were vehicle source,hydrocarbon volatile source,solvent source,industry source,biomass burning.The results obtained from the emission inventory in 2015 were the industry source,solvent source,vehicle source,fixed burning that contribute 35.5%,24.5%,28.9%,8.0%,respectively.Overall,the main sources of VOCs in the winter ambient air in Yibin City are vehicle,solvent and industry.
In order to understand the characteristics of volatile organic compounds in Yibin City in winter,air samples were collected at two sites in December 2016.Eighty-nine species of volatile organic compounds(VOCs)were measured by using pre-concentration-GC-MS method.This study investigated the volume fraction of VOCs and its ingredients.In addition,the main sources of VOCs were also identified.The results showed that the average volume fraction of VOCs was 35.10×10~(-9),and the highest volume fraction was 67.34×10~(-9)while the lowest volume fraction was 20.58×10~(-9).Aromatic hydrocarbons were the highest proportion in the monitored species category,followed by alkanes and halogenated hydrocarbons.Species with a large volume fraction were benzene,toluene,methyl chloride,dichloromethane,isobutene,isopropanol,n-butane and so on.Source apportionment for VOCs in Yibin City was taken by CMB model and emission inventory method.The CMB results indicated 6 major contribution sources of VOCs were vehicle source,hydrocarbon volatile source,solvent source,industry source,biomass burning.The results obtained from the emission inventory in 2015 were the industry source,solvent source,vehicle source,fixed burning that contribute 35.5%,24.5%,28.9%,8.0%,respectively.Overall,the main sources of VOCs in the winter ambient air in Yibin City are vehicle,solvent and industry.
引文
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[2]区家敏,冯小琼,刘郁葱,等.珠江三角洲机动车挥发性有机物排放化学成分谱研究[J].环境科学学报,2014,34(4):826-834.OU Jiamin, FENG Xiaoqiong, LIU Yucong, et al. Source characteristics of VOCs emissions from vehicular exhaust in the Pearl River Delta Region[J].Acta Scientiae Circumstantiae,2014,34(4):826-834.
[3]GUO H,CHENG H R,LING Z H,et al.Which emission sources are responsible for the volatile organic compounds in the atmosphere of Pearl River Delta[J]. Journal of Hazardous Materials,2011,118:116-124.
[4]BROWN S G,FRANKEL A,HAFNER H R.Source apportionment of VOCs in the Los Angeles Area using positive matrix factorization[J].Atmospheric Environment,2007,41(3):227-237.
[5]YANG L X,CHENG S H,WANG X F,et al.Source identification and health impact of PM2. 5in a heavily polluted urban atmosphere in China[J].Atmospheric Environment,2013,75:265-269.
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[7]BORBON A,CODDEVILLE P,LOCOGE N,et al. Characterising sources and sinks of rural VOC in eastern France[J].Chemosphere2004,57(8):931-942.
[8]刘雅婷,彭跃,白志鹏,等.沈阳市大气挥发性有机物(VOCs)污染特征[J].环境科学,2011,32(9):2777-2785.LIU Yating,PENG Yue,BAI Zhipeng,et al. Characterization of atmospheric volatile organic compounds in Shenyang,China[J].Environmental Science,2011,32(9):2777-2785.
[9]肖致美,毕晓辉,冯银厂,等.宁波市环境空气中PM10和PM2. 5来源解析[J].环境科学研究,2012,25(5):549-552.XIAO Zhimei,BI Xiaohui,FENG Yinchang,et al. Source apportionment of ambient PM10and PM2. 5in urban area of Ningbo City[J]. Research of Environmental Sciences,2012,25(5):549-552.
[10]WATSON J G,CHOW J C,FUJITA E M.Review of volatile organic compound source apportionment by chemical mass balance[J].Atmospheric Environment,1998,35:1567-1584.
[11]孙杰,王跃思,吴方堃,等.唐山市和北京市春夏秋季节大气VOCs组成及浓度变化[J].环境科学,2010,31(7):1438-1443.SUN Jie,WANG Yuesi,WU Fangkun,et al. Concentration and change of VOCs in summer and autumn in Tangshan[J].Environmental Science,2010,31(7):1438-1443.
[12]魏恩棋,时庭锐,李利荣.天津市大气中挥发性有机物的组成及分布特点[J].中国环境监测,2010,26(4):4-8.WEI Enqi,SHI Tingrui,LI Lirong,et al. The composition and distribution of VOCs in the atmosphere of Tianjin[J].Environmental Monitoring in China,2010,26(4):4-8.
[13]GENG F H,ZHAO C S,TANG X,et al. Analysis of ozone and VOCs measured in Shanghai:a case study[J]. Atmospheric Environment,2007,41(5):989-1001.
[14]GENG F H,TIE X X,XU J M,et al.Characteristics of ozone,NOx,and VOCs measured in Shanghai,China[J]. Atmospheric Environment,2008,42(29):6873-6883.
[15]王伯光,张远航,邵敏.珠江三角洲大气环境VOCs的时空分布特征[J],环境科学,2004,25(6):7-15.WANG Boguang,ZHANG Yuanhang,SHAO Min. Special and temporal distribution character of VOCs in the ambient air of Peal River Delta Region[J].Environmental Science,2004,25(6):7-15.
[16]MORINO Y,OHARA T,YOKOUCHI Y. Comprehensive source apportionment of volatile organic compounds using observational data,two receptor models,and an emission inventory in Tokyo metropolitan area[J]. Journal of Geophysical Research,2011. doi:10. 1029/2010jd014762.
[17]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,2006,26(5):757-763.LU Sihua,BAI Yuhua,ZHANG Guangshan,et al. Source apportionment of anthropogenic emissions of volatile organic compounds[J]. Acta Science Circumstantiae,2006,26(5):757-763.
[18]王伯光,张远航,邵敏.珠江三角洲大气环境VOCs的时空分布特征[J],环境科学,2004,25(6):7-15.WANG Boguang,ZHANG Yuanhang,SHAO Min. Special and temporal distribution character of VOCs in the ambient air of Peal River Delta Region[J].Environmental Science,2004,25(6):7-15.
[19]郑伟巍,毕晓辉,吴建会,等.宁波市大气挥发性有机物污染特征及关键活性组分[J].环境科学研究,2014,27(12):1412-1417.ZHENG Weiwei,BI Xiaohui,WU Jianhui,et al. Pollution characteristics and key reactive species of ambient VOCs in Ningbo City[J].Research of Environmental Sciences,2014,27(12):1412-1417.
[20]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&Physics,2015,15(12):6625-6636.
[21]JIA C,MAO X,HUANG T,et al. Non-methane hydrocarbons(NMHCs)and their contribution to ozone formation potential in a petrochemical industrialized city,northwest China[J]. Journal of Geophysical Research,2016,169:225-236.
[22]徐慧,张晗,邢振雨,等.厦门冬春季大气VOCs的污染特征及臭氧生成潜势[J].环境科学,2015,36(1):11-17.XU Hui,ZHANG Han,XING Zhenyu,et al.Pollution characteristics and ozone formation potential of ambient VOCs in winter and spring in Xiamen[J].Environmental Science,2015,36(1):11-17.
[23]罗达通,高健,王淑兰,等.上海秋季大气挥发性有机物特征及污染物来源分析[J].中国环境科学,2015,35(4):987-994.LUO Datong,GAO Jian,WANG Shulan,et al. Characteristics of volatile organic compounds and relative pollutants observed in autumn Shanghai[J].China Environmental Science,2015,35(4):987-994.
[24]林旭,朱彬,安俊琳,等.南京北郊VOCs对臭氧和二次有机气溶胶潜在贡献的研究[J].中国环境科学,2015,35(4):976-986.LIN Xu,ZHU Bin,AN Junlin,et al. Potential contribution of secondary organic aerosols and ozone of VOCs in the northern suburb of Nanjing[J].China Environmental Science,2015,35(4):976-986.
[25]WU R R,BO Y,LI J,et al. Method to establish the emission inventory of anthropogenic volatile organic compounds in China and its application in the period 2008-2012[J]. Atmospheric Environment,2016,127:244-254.
[26]MO Z W,SHAO M,LU S H,et al. Process-specific emission characteristics of volatile organic compounds(VOCs)from petrochemical facilities in the Yangtze River Delta,China[J].Science of the Total Environment,2015,533:422-431.
[27]SHI J W,DENG H,BAI Z P,et al. Emission and profile characteristic of volatile organic compounds emitted from coke production,iron smelt,heating station and power plant in Liaoning Province,China[J]. Science of the Total Environment,2015,515/516:101-108.
[28]LI X,WANG S,DUAN L,HAO J.Characterization of non-methane hydrocarbons emitted from open burning of wheat straw and corn stover in China[J]. Environmental Research Letters,2009. doi:10. 1088/1748-9326/4/4/044015.
[29]YUAN B,SHAO M,LU S H,et al.Source profiles of volatile organic compounds associated with solvent use in Beijing,China[J].Atmospheric Environment,2010,44(15):1919-1926.
[30]HE Z K,ZHANG Y P,WEI W J.Formaldehyde and VOC emissions at different manufacturing stages of wood-based panel[J]. Building and Environment,2012,47:197-204.
[31]ZHENG J Y,YU Y F,MO Z W,et al. Industrial sector-based volatile organic compound(VOC)source profiles measured in manufacturing facilities in the Pearl River Delta,China[J].Science of the Total Environment,2013,456/457(1):127-136.
[2]区家敏,冯小琼,刘郁葱,等.珠江三角洲机动车挥发性有机物排放化学成分谱研究[J].环境科学学报,2014,34(4):826-834.OU Jiamin, FENG Xiaoqiong, LIU Yucong, et al. Source characteristics of VOCs emissions from vehicular exhaust in the Pearl River Delta Region[J].Acta Scientiae Circumstantiae,2014,34(4):826-834.
[3]GUO H,CHENG H R,LING Z H,et al.Which emission sources are responsible for the volatile organic compounds in the atmosphere of Pearl River Delta[J]. Journal of Hazardous Materials,2011,118:116-124.
[4]BROWN S G,FRANKEL A,HAFNER H R.Source apportionment of VOCs in the Los Angeles Area using positive matrix factorization[J].Atmospheric Environment,2007,41(3):227-237.
[5]YANG L X,CHENG S H,WANG X F,et al.Source identification and health impact of PM2. 5in a heavily polluted urban atmosphere in China[J].Atmospheric Environment,2013,75:265-269.
[6]CHIANG H L,HWU C S,CHEN N S Y,et al.Emission factors and characteristics of criteria pollutant and volatile organic compounds(VOCs)in a freeway tunnel study[J]. Science of the Total Environment,2007,381(1/2/3):200-211.
[7]BORBON A,CODDEVILLE P,LOCOGE N,et al. Characterising sources and sinks of rural VOC in eastern France[J].Chemosphere2004,57(8):931-942.
[8]刘雅婷,彭跃,白志鹏,等.沈阳市大气挥发性有机物(VOCs)污染特征[J].环境科学,2011,32(9):2777-2785.LIU Yating,PENG Yue,BAI Zhipeng,et al. Characterization of atmospheric volatile organic compounds in Shenyang,China[J].Environmental Science,2011,32(9):2777-2785.
[9]肖致美,毕晓辉,冯银厂,等.宁波市环境空气中PM10和PM2. 5来源解析[J].环境科学研究,2012,25(5):549-552.XIAO Zhimei,BI Xiaohui,FENG Yinchang,et al. Source apportionment of ambient PM10and PM2. 5in urban area of Ningbo City[J]. Research of Environmental Sciences,2012,25(5):549-552.
[10]WATSON J G,CHOW J C,FUJITA E M.Review of volatile organic compound source apportionment by chemical mass balance[J].Atmospheric Environment,1998,35:1567-1584.
[11]孙杰,王跃思,吴方堃,等.唐山市和北京市春夏秋季节大气VOCs组成及浓度变化[J].环境科学,2010,31(7):1438-1443.SUN Jie,WANG Yuesi,WU Fangkun,et al. Concentration and change of VOCs in summer and autumn in Tangshan[J].Environmental Science,2010,31(7):1438-1443.
[12]魏恩棋,时庭锐,李利荣.天津市大气中挥发性有机物的组成及分布特点[J].中国环境监测,2010,26(4):4-8.WEI Enqi,SHI Tingrui,LI Lirong,et al. The composition and distribution of VOCs in the atmosphere of Tianjin[J].Environmental Monitoring in China,2010,26(4):4-8.
[13]GENG F H,ZHAO C S,TANG X,et al. Analysis of ozone and VOCs measured in Shanghai:a case study[J]. Atmospheric Environment,2007,41(5):989-1001.
[14]GENG F H,TIE X X,XU J M,et al.Characteristics of ozone,NOx,and VOCs measured in Shanghai,China[J]. Atmospheric Environment,2008,42(29):6873-6883.
[15]王伯光,张远航,邵敏.珠江三角洲大气环境VOCs的时空分布特征[J],环境科学,2004,25(6):7-15.WANG Boguang,ZHANG Yuanhang,SHAO Min. Special and temporal distribution character of VOCs in the ambient air of Peal River Delta Region[J].Environmental Science,2004,25(6):7-15.
[16]MORINO Y,OHARA T,YOKOUCHI Y. Comprehensive source apportionment of volatile organic compounds using observational data,two receptor models,and an emission inventory in Tokyo metropolitan area[J]. Journal of Geophysical Research,2011. doi:10. 1029/2010jd014762.
[17]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,2006,26(5):757-763.LU Sihua,BAI Yuhua,ZHANG Guangshan,et al. Source apportionment of anthropogenic emissions of volatile organic compounds[J]. Acta Science Circumstantiae,2006,26(5):757-763.
[18]王伯光,张远航,邵敏.珠江三角洲大气环境VOCs的时空分布特征[J],环境科学,2004,25(6):7-15.WANG Boguang,ZHANG Yuanhang,SHAO Min. Special and temporal distribution character of VOCs in the ambient air of Peal River Delta Region[J].Environmental Science,2004,25(6):7-15.
[19]郑伟巍,毕晓辉,吴建会,等.宁波市大气挥发性有机物污染特征及关键活性组分[J].环境科学研究,2014,27(12):1412-1417.ZHENG Weiwei,BI Xiaohui,WU Jianhui,et al. Pollution characteristics and key reactive species of ambient VOCs in Ningbo City[J].Research of Environmental Sciences,2014,27(12):1412-1417.
[20]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&Physics,2015,15(12):6625-6636.
[21]JIA C,MAO X,HUANG T,et al. Non-methane hydrocarbons(NMHCs)and their contribution to ozone formation potential in a petrochemical industrialized city,northwest China[J]. Journal of Geophysical Research,2016,169:225-236.
[22]徐慧,张晗,邢振雨,等.厦门冬春季大气VOCs的污染特征及臭氧生成潜势[J].环境科学,2015,36(1):11-17.XU Hui,ZHANG Han,XING Zhenyu,et al.Pollution characteristics and ozone formation potential of ambient VOCs in winter and spring in Xiamen[J].Environmental Science,2015,36(1):11-17.
[23]罗达通,高健,王淑兰,等.上海秋季大气挥发性有机物特征及污染物来源分析[J].中国环境科学,2015,35(4):987-994.LUO Datong,GAO Jian,WANG Shulan,et al. Characteristics of volatile organic compounds and relative pollutants observed in autumn Shanghai[J].China Environmental Science,2015,35(4):987-994.
[24]林旭,朱彬,安俊琳,等.南京北郊VOCs对臭氧和二次有机气溶胶潜在贡献的研究[J].中国环境科学,2015,35(4):976-986.LIN Xu,ZHU Bin,AN Junlin,et al. Potential contribution of secondary organic aerosols and ozone of VOCs in the northern suburb of Nanjing[J].China Environmental Science,2015,35(4):976-986.
[25]WU R R,BO Y,LI J,et al. Method to establish the emission inventory of anthropogenic volatile organic compounds in China and its application in the period 2008-2012[J]. Atmospheric Environment,2016,127:244-254.
[26]MO Z W,SHAO M,LU S H,et al. Process-specific emission characteristics of volatile organic compounds(VOCs)from petrochemical facilities in the Yangtze River Delta,China[J].Science of the Total Environment,2015,533:422-431.
[27]SHI J W,DENG H,BAI Z P,et al. Emission and profile characteristic of volatile organic compounds emitted from coke production,iron smelt,heating station and power plant in Liaoning Province,China[J]. Science of the Total Environment,2015,515/516:101-108.
[28]LI X,WANG S,DUAN L,HAO J.Characterization of non-methane hydrocarbons emitted from open burning of wheat straw and corn stover in China[J]. Environmental Research Letters,2009. doi:10. 1088/1748-9326/4/4/044015.
[29]YUAN B,SHAO M,LU S H,et al.Source profiles of volatile organic compounds associated with solvent use in Beijing,China[J].Atmospheric Environment,2010,44(15):1919-1926.
[30]HE Z K,ZHANG Y P,WEI W J.Formaldehyde and VOC emissions at different manufacturing stages of wood-based panel[J]. Building and Environment,2012,47:197-204.
[31]ZHENG J Y,YU Y F,MO Z W,et al. Industrial sector-based volatile organic compound(VOC)source profiles measured in manufacturing facilities in the Pearl River Delta,China[J].Science of the Total Environment,2013,456/457(1):127-136.
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