天津隧道机动车VOCs污染特征与排放因子
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摘要
应用隧道测试方法在天津市五经路隧道于工作日和非工作日对机动车挥发性有机物(VOCs)污染特征及排放因子(EFs)进行研究,采用3.2 L真空采样罐采集隧道内气体样品,应用气相色谱-质谱联用仪(GC-MS)对罐内VOCs组分进行分析,得到99种组分的定量结果.对VOCs浓度水平与变化特征、EFs进行了分析,计算隧道内VOCs的臭氧生成潜势(OFPs)和二次有机气溶胶生成潜势(SOAFPs),并与已发表的研究数据进行了对比.结果表明,隧道入口VOCs平均浓度为(190.85±51.15)μg·m~(-3),中点平均浓度为(257.44±62.02)μg·m~(-3).隧道总排放因子为(45.12±10.97) mg·(km·辆)-1,烷烃、烯烃、炔烃、芳香烃、卤代烃和含氧VOCs(OVOCs)的EFs分别为(22.79±7.15)、(5.04±1.20)、(0.78±0.34)、(9.86±2.81)、(0.26±0.17)和(6.25±2.27) mg·(km·辆)-1,与2009年测试结果相比下降明显.其中,异戊烷、甲苯、乙烯、甲基叔丁基醚(MTBE)和乙烷是机动车排放VOCs中排放因子较高的组分;甲基叔丁基醚/苯(MTBE/B)、甲基叔丁基醚/甲苯(MTBE/T)比值分别为1.07和0.77,说明蒸发排放对机动车排放VOCs的贡献不可忽视.隧道内VOCs的OFPs和SOAFPs分别为(145.50±37.85) mg·(km·辆)-1和(43.87±12.75) mg·(km·辆)-1,较2009年天津测试结果分别降低94.23%和90.88%,OFPs和SOAFPs的锐减与排放标准加严和油品升级密切相关.
The pollution characteristics and emission factors(EFs) of the volatile organic compounds(VOCs) of vehicles were investigated using the tunnel test method on weekdays and weekends in the Wujinglu Tunnel in Tianjin,China.Gas samples in the tunnel were collected with 3.2 L stainless steel canisters and 99 VOCs species were analyzed by gas chromatography-mass spectrometry(GC-MS).The concentration levels,variation characteristics,and EFs of the VOCs were analyzed.The ozone formation potentials(OFPs) and secondary organic aerosol formation potentials(SOAFPs) of the VOCs in the tunnel were calculated.Moreover,a comparison of the study results with current literature was conducted.The total concentrations of VOCs at the inlet and midpoint are(190.85 ± 51.15) μg·m~(-3) and(257.44 ± 62.02) μg·m~(-3),respectively.The total EFs are(45.12 ± 10.97) mg·(km·veh)-1 and the EFs for alkanes,alkenes,alkynes,aromatics,halocarbons,and oxygenated volatile organic compounds(OVOCs) are(22.79 ±7.15),(5.04 ± 1.20),(0.78 ± 0.34),(9.86 ± 2.81),(0.26 ± 0.17),and(6.25 ± 2.27) mg·(km·veh)-1,respectively.They are notably smaller than the values obtained in a previous test in 2009.Isopentane,toluene,ethylene,methyl tert-butyl ether(MTBE),and ethane were the top five species among the VOC EFs.The ratios of methyl tert-butyl ether/benzene(MTBE/B) and methyl tert-butyl ether/toluene(MTBE/T) are 1.07 and 0.77,respectively.This implies that the contribution of evaporative emissions from vehicles to VOCs emissions cannot be ignored.The OFPs and SOAFPs in the tunnel are(145.50 ± 37.85) and(43.87 ± 12.75)mg·(km·veh)-1,respectively.Compared with the test in 2009,the OFPs and SOAFPs are 94.23% and 90.88% smaller,respectively.The sharp decrease of the OFPs and SOAFPs is closely related to stricter emission standards and the upgrade of oil products.
The pollution characteristics and emission factors(EFs) of the volatile organic compounds(VOCs) of vehicles were investigated using the tunnel test method on weekdays and weekends in the Wujinglu Tunnel in Tianjin,China.Gas samples in the tunnel were collected with 3.2 L stainless steel canisters and 99 VOCs species were analyzed by gas chromatography-mass spectrometry(GC-MS).The concentration levels,variation characteristics,and EFs of the VOCs were analyzed.The ozone formation potentials(OFPs) and secondary organic aerosol formation potentials(SOAFPs) of the VOCs in the tunnel were calculated.Moreover,a comparison of the study results with current literature was conducted.The total concentrations of VOCs at the inlet and midpoint are(190.85 ± 51.15) μg·m~(-3) and(257.44 ± 62.02) μg·m~(-3),respectively.The total EFs are(45.12 ± 10.97) mg·(km·veh)-1 and the EFs for alkanes,alkenes,alkynes,aromatics,halocarbons,and oxygenated volatile organic compounds(OVOCs) are(22.79 ±7.15),(5.04 ± 1.20),(0.78 ± 0.34),(9.86 ± 2.81),(0.26 ± 0.17),and(6.25 ± 2.27) mg·(km·veh)-1,respectively.They are notably smaller than the values obtained in a previous test in 2009.Isopentane,toluene,ethylene,methyl tert-butyl ether(MTBE),and ethane were the top five species among the VOC EFs.The ratios of methyl tert-butyl ether/benzene(MTBE/B) and methyl tert-butyl ether/toluene(MTBE/T) are 1.07 and 0.77,respectively.This implies that the contribution of evaporative emissions from vehicles to VOCs emissions cannot be ignored.The OFPs and SOAFPs in the tunnel are(145.50 ± 37.85) and(43.87 ± 12.75)mg·(km·veh)-1,respectively.Compared with the test in 2009,the OFPs and SOAFPs are 94.23% and 90.88% smaller,respectively.The sharp decrease of the OFPs and SOAFPs is closely related to stricter emission standards and the upgrade of oil products.
引文
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[7]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(2):223-237.
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[11]Franco V,Kousoulidou M,Muntean M,et al.Road vehicle emission factors development:a review[J].Atmospheric Environment,2013,70:84-97.
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[13]Chiang H L,Hwu C S,Chen S Y,et al.Emission factors and characteristics of criteria pollutants and volatile organic compounds(VOCs)in a freeway tunnel study[J].Science of the Total Environment,2007,381(1-3):200-211.
[14]付琳琳,邵敏,刘源,等.机动车VOCs排放特征和排放因子的隧道测试研究[J].环境科学学报,2005,25(7):879-885.Fu L,Shao M,Liu Y,et al.Tunnel experimental study on the emission factors of volatile organic compounds(VOCs)from vehicles[J].Acta Scientiae Circumstantiae,2005,25(7):879-885.
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[16]Zhang Y L,Yang W Q,Simpson I,et al.Decadal changes in emissions of volatile organic compounds(VOCs)from on-road vehicles with intensified automobile pollution control:Case study in a busy urban tunnel in south China[J].Environmental Pollution,2018,233:806-819.
[17]Zhang Q J,Wu L,Fang X Z,et al.Emission factors of volatile organic compounds(VOCs)based on the detailed vehicle classification in a tunnel study[J].Science of the Total Environment,2017,624:878-886.
[18]Cui L,Wang X L,Ho K F,et al.Decrease of VOC emissions from vehicular emissions in Hong Kong from 2003 to 2015:results from a tunnel study[J].Atmospheric Environment,2018,177:64-74.
[19]王玮,梁宝生,曾凡刚,等.谭裕沟隧道VOCs污染特征和排放因子研究[J].环境科学研究,2001,14(4):9-12.Wang W,Liang B S,Zeng F G,et al.Study on pollution characteristics and emission factors of volatile organic compounds(VOCs)in Tanyugou highway tunnel[J].Research of Environmental Sciences,2001,14(4):9-12.
[20]于艳,王秀艳,杨文.天津市机动车二次有机气溶胶生成潜势的估算[J].中国环境科学,2015,35(2):381-386.Yu Y,Wang X Y,Yang W.Estimate of vehicles generation of secondary organic aerosols of Tianjin[J].China Environmental Science,2015,35(2):381-386.
[21]王伯光,邵敏,张远航,等.机动车排放中挥发性有机污染物的组成及其特征研究[J].环境科学研究,2006,19(6):75-80.Wang B G,Shao M,Zhang Y H,et al.A study of volatile organic compounds and its emission factors from city vehicles[J].Research of Environmental Sciences,2006,19(6):75-80.
[22]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 X,Zhu B,An J L,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.
[23]张启钧,吴琳,刘明月,等.南京市机动车排放VOCs的污染特征与健康风险评价[J].中国环境科学,2016,36(10):3118-3125.Zhang Q J,Wu L,Liu M Y,et al.Pollution characteristics and health risk assessment of VOCs from vehicle exhaust in Nanjing,China[J].China Environmental Science,2016,36(10):3118-3125.
[24]Dong D,Shao M,Li Y,et al.Carbonyl emissions from heavyduty diesel vehicle exhaust in China and the contribution to ozone formation potential[J].Journal of Environmental Sciences,2014,26(1):122-128.
[25]陈天增,葛艳丽,刘永春,等.我国机动车排放VOCs及其大气环境影响[J].环境科学,2018,39(2):478-492.Chen T Z,Ge Y L,Liu Y C,et al.VOCs emission from motor vehicles in China and its impact on the atmospheric environment[J].Environmental Science,2018,39(2):478-492.
[26]葛卫华,金陶胜.香港小汽车和出租车非甲烷碳氢排放特性研究[J].资源节约与环保,2015,(1):74-75.
[27]Tang J H,Chan L Y,Chan C Y,et al.Implications of changing urban and rural emissions on non-methane hydrocarbons in the Pearl River Delta region of China[J].Atmospheric Environment,2008,42(16):3780-3794.
[28]Liu H,Man H Y,Tschantz M,et al.VOC from vehicular evaporation emissions:status and control strategy[J].Environmental Science&Technology,2015,49(24):14424-14431.
[29]Yue T T,Yue X,Chai F H,et al.Characteristics of volatile organic compounds(VOCs)from the evaporative emissions of modern passenger cars[J].Atmospheric Environment,2017,151:62-69.
[30]Zhang Y L,Wang X M,Zhang Z,et al.Species profiles and normalized reactivity of volatile organic compounds from gasoline evaporation in China[J].Atmospheric Environment,2013,79:110-118.
[31]Schauer J J,Kleeman M J,Cass G R,et al.Measurement of emissions from air pollution sources.5.C1-C32organic compounds from gasoline-powered motor vehicles[J].Environmental Science&Technology,2002,36(6):1169-1180.
[32]Yao Z L,Shen X B,Ye Y,et al.On-road emission characteristics of VOCs from diesel trucks in Beijing,China[J].Atmospheric Environment,2015,103:87-93.
[33]Carter W P L.Updated maximum incremental reactivity scale and hydrocarbon bin reactivities for regulatory applications[R].California:California Air Resources Board,2009.
[34]Grosjean D,Seinfeld J H.Parameterization of the formation potential of secondary organic aerosols[J].Atmospheric Environment,1989,23(8):1733-1747.
[35]Grosjean D.In situ organic aerosol formation during a smog episode:estimated production and chemical functionality[J].Atmospheric Environment.Part A.General Topics,1992,26(6):953-963.
[36]吕子峰,郝吉明,段菁春,等.北京市夏季二次有机气溶胶生成潜势的估算[J].环境科学,2009,30(4):969-975.LüZ F,Hao J M,Duan J C,et al.Estimate of the formation potential of secondary organic aerosol in Beijing summertime[J].Environmental Science,2009,30(4):969-975.
[37]郭和军.汽油品质对车辆尾气排放影响研究[D].武汉:武汉理工大学,2005.
[2]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.
[3]Wang H L,Jing S A,Lou S R,et al.Volatile organic compounds(VOCs)source profiles of on-road vehicle emissions in China[J].Science of the Total Environment,2017,607-608:253-261.
[4]Guenther A,Hewitt C N,Erickson D,et al.A global model of natural volatile organic compound emissions[J].Journal of Geophysical Research:Atmospheres,1995,100(D5):8873-8892.
[5]Atkinson R,Arey J.Atmospheric degradation of volatile organic compounds[J].Chemical Reviews,2003,103(12):4605-4638.
[6]Han M,Lu X Q,Zhao C S,et al.Characterization and source apportionment of volatile organic compounds in urban and suburban Tianjin,China[J].Advances in Atmospheric Sciences,2015,32(3):439-444.
[7]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(2):223-237.
[8]Zhao B,Wang P,Ma J Z,et al.A high-resolution emission inventory of primary pollutants for the Huabei region,China[J].Atmospheric Chemistry and Physics,2012,12(1):481-501.
[9]中华人民共和国环境保护部.中国机动车环境管理年报[R].北京:中华人民共和国环境保护部,2017.
[10]公安部交通管理局.2016年全国机动车和驾驶人保持快速增长新登记汽车2752万辆新增驾驶人3314万人[DB/OL].http://www.sohu.com/a/123961699_341502,2017-01-10.
[11]Franco V,Kousoulidou M,Muntean M,et al.Road vehicle emission factors development:a review[J].Atmospheric Environment,2013,70:84-97.
[12]Hwa M Y,Hsieh C C,Wu T C,et al.Real-world vehicle emissions and VOCs profile in the Taipei tunnel located at Taiwan Taipei area[J].Atmospheric Environment,2002,36(12):1993-2002.
[13]Chiang H L,Hwu C S,Chen S Y,et al.Emission factors and characteristics of criteria pollutants and volatile organic compounds(VOCs)in a freeway tunnel study[J].Science of the Total Environment,2007,381(1-3):200-211.
[14]付琳琳,邵敏,刘源,等.机动车VOCs排放特征和排放因子的隧道测试研究[J].环境科学学报,2005,25(7):879-885.Fu L,Shao M,Liu Y,et al.Tunnel experimental study on the emission factors of volatile organic compounds(VOCs)from vehicles[J].Acta Scientiae Circumstantiae,2005,25(7):879-885.
[15]王伯光,张远航,祝昌健,等.城市机动车排放因子隧道试验研究[J].环境科学,2001,22(2):55-59.Wang B G,Zhang Y H,Zhu C J,et al.A study on city motor vehicle emission factors by tunnel test[J].Environmental Science,2001,22(2):55-59.
[16]Zhang Y L,Yang W Q,Simpson I,et al.Decadal changes in emissions of volatile organic compounds(VOCs)from on-road vehicles with intensified automobile pollution control:Case study in a busy urban tunnel in south China[J].Environmental Pollution,2018,233:806-819.
[17]Zhang Q J,Wu L,Fang X Z,et al.Emission factors of volatile organic compounds(VOCs)based on the detailed vehicle classification in a tunnel study[J].Science of the Total Environment,2017,624:878-886.
[18]Cui L,Wang X L,Ho K F,et al.Decrease of VOC emissions from vehicular emissions in Hong Kong from 2003 to 2015:results from a tunnel study[J].Atmospheric Environment,2018,177:64-74.
[19]王玮,梁宝生,曾凡刚,等.谭裕沟隧道VOCs污染特征和排放因子研究[J].环境科学研究,2001,14(4):9-12.Wang W,Liang B S,Zeng F G,et al.Study on pollution characteristics and emission factors of volatile organic compounds(VOCs)in Tanyugou highway tunnel[J].Research of Environmental Sciences,2001,14(4):9-12.
[20]于艳,王秀艳,杨文.天津市机动车二次有机气溶胶生成潜势的估算[J].中国环境科学,2015,35(2):381-386.Yu Y,Wang X Y,Yang W.Estimate of vehicles generation of secondary organic aerosols of Tianjin[J].China Environmental Science,2015,35(2):381-386.
[21]王伯光,邵敏,张远航,等.机动车排放中挥发性有机污染物的组成及其特征研究[J].环境科学研究,2006,19(6):75-80.Wang B G,Shao M,Zhang Y H,et al.A study of volatile organic compounds and its emission factors from city vehicles[J].Research of Environmental Sciences,2006,19(6):75-80.
[22]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 X,Zhu B,An J L,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.
[23]张启钧,吴琳,刘明月,等.南京市机动车排放VOCs的污染特征与健康风险评价[J].中国环境科学,2016,36(10):3118-3125.Zhang Q J,Wu L,Liu M Y,et al.Pollution characteristics and health risk assessment of VOCs from vehicle exhaust in Nanjing,China[J].China Environmental Science,2016,36(10):3118-3125.
[24]Dong D,Shao M,Li Y,et al.Carbonyl emissions from heavyduty diesel vehicle exhaust in China and the contribution to ozone formation potential[J].Journal of Environmental Sciences,2014,26(1):122-128.
[25]陈天增,葛艳丽,刘永春,等.我国机动车排放VOCs及其大气环境影响[J].环境科学,2018,39(2):478-492.Chen T Z,Ge Y L,Liu Y C,et al.VOCs emission from motor vehicles in China and its impact on the atmospheric environment[J].Environmental Science,2018,39(2):478-492.
[26]葛卫华,金陶胜.香港小汽车和出租车非甲烷碳氢排放特性研究[J].资源节约与环保,2015,(1):74-75.
[27]Tang J H,Chan L Y,Chan C Y,et al.Implications of changing urban and rural emissions on non-methane hydrocarbons in the Pearl River Delta region of China[J].Atmospheric Environment,2008,42(16):3780-3794.
[28]Liu H,Man H Y,Tschantz M,et al.VOC from vehicular evaporation emissions:status and control strategy[J].Environmental Science&Technology,2015,49(24):14424-14431.
[29]Yue T T,Yue X,Chai F H,et al.Characteristics of volatile organic compounds(VOCs)from the evaporative emissions of modern passenger cars[J].Atmospheric Environment,2017,151:62-69.
[30]Zhang Y L,Wang X M,Zhang Z,et al.Species profiles and normalized reactivity of volatile organic compounds from gasoline evaporation in China[J].Atmospheric Environment,2013,79:110-118.
[31]Schauer J J,Kleeman M J,Cass G R,et al.Measurement of emissions from air pollution sources.5.C1-C32organic compounds from gasoline-powered motor vehicles[J].Environmental Science&Technology,2002,36(6):1169-1180.
[32]Yao Z L,Shen X B,Ye Y,et al.On-road emission characteristics of VOCs from diesel trucks in Beijing,China[J].Atmospheric Environment,2015,103:87-93.
[33]Carter W P L.Updated maximum incremental reactivity scale and hydrocarbon bin reactivities for regulatory applications[R].California:California Air Resources Board,2009.
[34]Grosjean D,Seinfeld J H.Parameterization of the formation potential of secondary organic aerosols[J].Atmospheric Environment,1989,23(8):1733-1747.
[35]Grosjean D.In situ organic aerosol formation during a smog episode:estimated production and chemical functionality[J].Atmospheric Environment.Part A.General Topics,1992,26(6):953-963.
[36]吕子峰,郝吉明,段菁春,等.北京市夏季二次有机气溶胶生成潜势的估算[J].环境科学,2009,30(4):969-975.LüZ F,Hao J M,Duan J C,et al.Estimate of the formation potential of secondary organic aerosol in Beijing summertime[J].Environmental Science,2009,30(4):969-975.
[37]郭和军.汽油品质对车辆尾气排放影响研究[D].武汉:武汉理工大学,2005.
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