珠江三角洲轻型汽油车匀速状态挥发性有机物排放特征研究
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摘要
以18辆轻型汽油车(LDGVs)为研究对象,利用底盘测功机搭建挥发性有机物(VOCs)采样系统.利用气相色谱-质谱仪(GC-MS)和高效液相色谱(HPLC)识别了匀速25 km·h~(-1)时尾气VOCs化学成分谱和排放因子,并在分析时考虑了排放标准、行驶工况和车辆属性等因素的影响.结果表明,轻型汽油车低速匀速工况下尾气组成以烷烃(40.8%,C_5～C_7烷烃较多)为主,其次是芳香烃(29.5%)和含氧VOCs(26.0%),烯炔烃(3.6%)和卤代烃(0.1%)较少.其中,甲醛、异戊烷、甲苯、苯、间/对二甲苯、丙酮、2-甲基戊烷、正戊烷、1,2,4-三甲基苯和壬醛是比例最高的物质(52.01%).低速匀速行驶中生成了比例更低的烯烃和比例更高的C_5～C_7烷烃和OVOCs.排放标准为国III、IV和V的轻型汽油车在低速匀速工况下,VOCs排放因子分别为(50.12±46.83)、(40.26±31.15)和(3.25±0.65) mg·km~(-1).国IV到国V车的烷烃、烯炔烃、芳香烃、卤代烃和总VOCs降幅均超过88%,而OVOCs降幅只有约55%,说明OVOCs在国V车的排放富集程度更高.总体来讲,国V车排放的VOCs反应活性约为国IV车排放的VOCs反应活性的11%.车辆属性对VOCs排放的影响表现为:年份、里程和排量的增加会促进VOCs排放的整体增加,而基准质量对VOCs排放的影响相对较小.
In this study, VOCs(volatile organic compounds) emissions from 18 light-duty gasoline-fueled vehicles(LDGV) were measured by VOCs sampling system based on chassis dynamometer. The VOCs source profiles and emission factors of LDGV at a constant speed of 25 km·h~(-1) were identified by GC-MS(Gas Chromatography-Mass Spectrometer) and HPLC(High Performance Liquid Chromatography), and the effects of emission standard, driving conditions and vehicle attributes were considered in the analysis. At low constant speed, the VOCs compositions of LDGV were mainly alkanes(40.8%, mainly C_5～C_7 alkanes), followed by aromatics(29.5%) and OVOCs(26.0%), with less alkynes(3.6%) and halohydrocarbon(0.1%). Formaldehyde, isopentane, toluene, benzene, m/p-xylene, acetone, 2-methyl-pentane, n-pentane, 1,2,4-trimethylbenzene and nonaldehydes were the top10 substances(52.01%). Lower alkenes but higher C_5～C_7 alkanes and OVOCs were generated during low constant speed driving. At low constant speed, the total VOCs emission factors of China III, IV and V vehicles were(50.12±46.83),(40.26±31.15) and(3.25±0.65) mg·km~(-1). Reductions of alkanes, alkenes and alkynes, aromatics, halohydrocarbon and total VOCs were all higher than 88% from China IV to China V, while that of OVOCs is only around 55%, which demonstrated higher OVOCs enrichment in China V vehicles. Overall, the total VOCs reactivity from China V vehicle emissions was around 11% of that from China IV vehicle emissions. Meanwhile VOCs emission was also affected by vehicle attributes:the increase of years, mileages and displacement led to increases in VOCs while the reference mass had less impacts.
In this study, VOCs(volatile organic compounds) emissions from 18 light-duty gasoline-fueled vehicles(LDGV) were measured by VOCs sampling system based on chassis dynamometer. The VOCs source profiles and emission factors of LDGV at a constant speed of 25 km·h~(-1) were identified by GC-MS(Gas Chromatography-Mass Spectrometer) and HPLC(High Performance Liquid Chromatography), and the effects of emission standard, driving conditions and vehicle attributes were considered in the analysis. At low constant speed, the VOCs compositions of LDGV were mainly alkanes(40.8%, mainly C_5～C_7 alkanes), followed by aromatics(29.5%) and OVOCs(26.0%), with less alkynes(3.6%) and halohydrocarbon(0.1%). Formaldehyde, isopentane, toluene, benzene, m/p-xylene, acetone, 2-methyl-pentane, n-pentane, 1,2,4-trimethylbenzene and nonaldehydes were the top10 substances(52.01%). Lower alkenes but higher C_5～C_7 alkanes and OVOCs were generated during low constant speed driving. At low constant speed, the total VOCs emission factors of China III, IV and V vehicles were(50.12±46.83),(40.26±31.15) and(3.25±0.65) mg·km~(-1). Reductions of alkanes, alkenes and alkynes, aromatics, halohydrocarbon and total VOCs were all higher than 88% from China IV to China V, while that of OVOCs is only around 55%, which demonstrated higher OVOCs enrichment in China V vehicles. Overall, the total VOCs reactivity from China V vehicle emissions was around 11% of that from China IV vehicle emissions. Meanwhile VOCs emission was also affected by vehicle attributes:the increase of years, mileages and displacement led to increases in VOCs while the reference mass had less impacts.
引文
Cao X Y,Yao Z L,Shen X B,et al.2016.On-road emission characteristics of VOCs from light-duty gasoline vehicles in Beijing,China[J].Atmospheric Environment,124:146-155
Carter W P L.2008.Reactivity estimates for selected consumer product compounds[R].California:Center for Environmental Research and Technology,College of Engineering,University of California
车汶蔚,郑君瑜,钟流举.2009.珠江三角洲机动车污染物排放特征及分担率[J].环境科学研究,22(4):456-461
Dai T Y,Wang W,Ren L H,et al.2009.Emissions of non-methane hydrocarbons from cars in China[J].Science China,53(1):263-272
丁嘉磊,张铁臣,高俊华,等.2018.轻型汽油车不同工况下NMOG的排放特性研究[J].实验科学与技术,16(2):30-36
付琳琳.2005.大气挥发性有机物(VOCs)人为源排放特征研究[D].北京:北京大学
高爽,金亮茂,史建武,等.2012.轻型汽油车VOCs排放特征和排放因子台架测试研究[J].中国环境科学,32(3):397-405
广东省环境监测中心,香港特别行政区环境保护署.2007—2017.粤港澳珠江三角洲区域空气监测网络2007年监测结果报告[R].PRDAIR-2007-2.粤港澳珠江三角洲区域空气监测网络2017年监测结果报告[R].PRDAIR-2017-5.广州+香港:广东省环境监测中心+香港特别行政区环境保护署.1-27; 1-38
广东省统计局.2006—2016.广东省统计年鉴[M].北京:中国统计出版社
Guo H,Zou S C,Tsai W Y,et al.2011.Emission characteristics of nonmethane hydrocarbons from private cars and taxis at different driving speeds in Hong Kong[J].Atmospheric Environment,45:2711-2721
国家能源部.2017.关于扩大生物燃料乙醇生产和推广使用车用乙醇汽油的实施方案[R].发改能源[2017]1508号.北京:国家能源部
何学良,李疏松.1990.内燃机燃烧学[M].北京:机械工业出版社
Huang Y,Ho S S H,Ho K F,et al.2011.Characteristics and health impacts of VOCs and carbonyls associated with residential cooking activities in Hong Kong[J].Journal of Hazardous Materials,186:344-351
卢清.2013.珠江三角洲地区人为源VOCs 排放特征及时空分配改进研究[D].广州:华南理工大学
Kassomenos P A,Dimitriou K,Paschalidou A K.2013.Human health damage caused by particulate matter PM10 and ozone in urban environments:the case of Athens,Greece[J].Environmental Monitoring & Assessment,185(8):6933-6942
Kleinman L I,Daum P H,Lee Y,et al.2002.Ozone production efficiency in an urban area[J].Journal of Geophysical Research Atmospheres,107(D23),DOI:10.1029/2002jd002529
区家敏,冯小琼,刘郁葱,等.2014.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,34(4):826-834
Ou J M,Zheng J Y,Li R R,et al.2011.Emission characteristics of nonmethane hydrocarbons from private cars and taxis at different driving speeds in Hong Kong[J].Atmospheric Environment,45:2711-2721
Ou J,Yuan Z B,Zheng J Y,et al.Ambient ozone control in a photochemically active region:short-term despiking or long-term attainment?[J].Environmental Science & Technology,50(11):5720
潘月云,李楠,郑君瑜,等.2015.广东省人为源大气污染物排放清单及特征研究[J].环境科学学报,35(9):2655-2669
Pang X B,Mu Y J,Yuan J,et al.2008.Carbonyls emission from ethanol-blended gasoline and biodiesel-ethanol-diesel used in engines[J].Atmospheric Environment,42:1349-1358
Peng G,Zhang H,Yang S C,et al.2015.Comparative study on measurements of formaldehyde emission of methanol/gasoline fueled SI engine[J].Fuel,148:9-15
乔月珍,王红丽,黄成,等.2012.机动车尾气排放VOCs源成分谱及其大气反应活性[J].环境科学,33(4):1071-1080
Wang H L,Jing S A,Lou S R,et al.2017.Volatile organic compounds (VOCs) source profiles of on-road vehicle emissions in China.[J].Science of the Total Environment,607-608:253-261
Wang J,Jin L M,Gao J H,et al.2013.Investigation of speciated VOC in gasoline vehicular exhaust under ECE and EUDC test cycles[J].Science of the Total Environment,445-446:110-116
王阳.2008.烃类燃料的预混层流火焰燃烧特性研究[D].天津:天津大学
Yang Y D,Shao M,Keel S,et al.How the OH reactivity affects the ozone production efficiency:case studies in Beijing and Heshan,China[J].Atmospheric Chemistry and Physics,17:7127-7142
Yuan Z B,Zhong L J,Lau A K H, et al.2012.Volatile organic compounds in the Pearl River Delta:Identification of source regions and recommendations for emission-oriented monitoring strategies[J].Atmospheric Environment,76:162-172
张凡,王建海,杨正军,等.2012.使用FTIR、HPLC、GC-MS 联合测量甲醇汽油车的非常规污染物排放[C].中国内燃机学会燃烧节能净化分会学术年会.南宁:1-6
张铁臣,宋崇林,范嘉睿,等.2008.汽油车挥发性有机物排放特性的研究[J].工程热物理学报,29(4):703-706
Zheng J Y,Zhong L J,Che W W,et al.2009a.A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta Region,China,and its uncer-tainty assessment[J].Atmospheric Environmental,43:5112-5122
Zheng J Y,Shao M,Che W W,et al.2009b.Speciated VOC emission inventory and spatial patterns of ozone formation potential in the Pearl River Delta,China[J].Environmental Science and Technology,43:8580-8586
Carter W P L.2008.Reactivity estimates for selected consumer product compounds[R].California:Center for Environmental Research and Technology,College of Engineering,University of California
车汶蔚,郑君瑜,钟流举.2009.珠江三角洲机动车污染物排放特征及分担率[J].环境科学研究,22(4):456-461
Dai T Y,Wang W,Ren L H,et al.2009.Emissions of non-methane hydrocarbons from cars in China[J].Science China,53(1):263-272
丁嘉磊,张铁臣,高俊华,等.2018.轻型汽油车不同工况下NMOG的排放特性研究[J].实验科学与技术,16(2):30-36
付琳琳.2005.大气挥发性有机物(VOCs)人为源排放特征研究[D].北京:北京大学
高爽,金亮茂,史建武,等.2012.轻型汽油车VOCs排放特征和排放因子台架测试研究[J].中国环境科学,32(3):397-405
广东省环境监测中心,香港特别行政区环境保护署.2007—2017.粤港澳珠江三角洲区域空气监测网络2007年监测结果报告[R].PRDAIR-2007-2.粤港澳珠江三角洲区域空气监测网络2017年监测结果报告[R].PRDAIR-2017-5.广州+香港:广东省环境监测中心+香港特别行政区环境保护署.1-27; 1-38
广东省统计局.2006—2016.广东省统计年鉴[M].北京:中国统计出版社
Guo H,Zou S C,Tsai W Y,et al.2011.Emission characteristics of nonmethane hydrocarbons from private cars and taxis at different driving speeds in Hong Kong[J].Atmospheric Environment,45:2711-2721
国家能源部.2017.关于扩大生物燃料乙醇生产和推广使用车用乙醇汽油的实施方案[R].发改能源[2017]1508号.北京:国家能源部
何学良,李疏松.1990.内燃机燃烧学[M].北京:机械工业出版社
Huang Y,Ho S S H,Ho K F,et al.2011.Characteristics and health impacts of VOCs and carbonyls associated with residential cooking activities in Hong Kong[J].Journal of Hazardous Materials,186:344-351
卢清.2013.珠江三角洲地区人为源VOCs 排放特征及时空分配改进研究[D].广州:华南理工大学
Kassomenos P A,Dimitriou K,Paschalidou A K.2013.Human health damage caused by particulate matter PM10 and ozone in urban environments:the case of Athens,Greece[J].Environmental Monitoring & Assessment,185(8):6933-6942
Kleinman L I,Daum P H,Lee Y,et al.2002.Ozone production efficiency in an urban area[J].Journal of Geophysical Research Atmospheres,107(D23),DOI:10.1029/2002jd002529
区家敏,冯小琼,刘郁葱,等.2014.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,34(4):826-834
Ou J M,Zheng J Y,Li R R,et al.2011.Emission characteristics of nonmethane hydrocarbons from private cars and taxis at different driving speeds in Hong Kong[J].Atmospheric Environment,45:2711-2721
Ou J,Yuan Z B,Zheng J Y,et al.Ambient ozone control in a photochemically active region:short-term despiking or long-term attainment?[J].Environmental Science & Technology,50(11):5720
潘月云,李楠,郑君瑜,等.2015.广东省人为源大气污染物排放清单及特征研究[J].环境科学学报,35(9):2655-2669
Pang X B,Mu Y J,Yuan J,et al.2008.Carbonyls emission from ethanol-blended gasoline and biodiesel-ethanol-diesel used in engines[J].Atmospheric Environment,42:1349-1358
Peng G,Zhang H,Yang S C,et al.2015.Comparative study on measurements of formaldehyde emission of methanol/gasoline fueled SI engine[J].Fuel,148:9-15
乔月珍,王红丽,黄成,等.2012.机动车尾气排放VOCs源成分谱及其大气反应活性[J].环境科学,33(4):1071-1080
Wang H L,Jing S A,Lou S R,et al.2017.Volatile organic compounds (VOCs) source profiles of on-road vehicle emissions in China.[J].Science of the Total Environment,607-608:253-261
Wang J,Jin L M,Gao J H,et al.2013.Investigation of speciated VOC in gasoline vehicular exhaust under ECE and EUDC test cycles[J].Science of the Total Environment,445-446:110-116
王阳.2008.烃类燃料的预混层流火焰燃烧特性研究[D].天津:天津大学
Yang Y D,Shao M,Keel S,et al.How the OH reactivity affects the ozone production efficiency:case studies in Beijing and Heshan,China[J].Atmospheric Chemistry and Physics,17:7127-7142
Yuan Z B,Zhong L J,Lau A K H, et al.2012.Volatile organic compounds in the Pearl River Delta:Identification of source regions and recommendations for emission-oriented monitoring strategies[J].Atmospheric Environment,76:162-172
张凡,王建海,杨正军,等.2012.使用FTIR、HPLC、GC-MS 联合测量甲醇汽油车的非常规污染物排放[C].中国内燃机学会燃烧节能净化分会学术年会.南宁:1-6
张铁臣,宋崇林,范嘉睿,等.2008.汽油车挥发性有机物排放特性的研究[J].工程热物理学报,29(4):703-706
Zheng J Y,Zhong L J,Che W W,et al.2009a.A highly resolved temporal and spatial air pollutant emission inventory for the Pearl River Delta Region,China,and its uncer-tainty assessment[J].Atmospheric Environmental,43:5112-5122
Zheng J Y,Shao M,Che W W,et al.2009b.Speciated VOC emission inventory and spatial patterns of ozone formation potential in the Pearl River Delta,China[J].Environmental Science and Technology,43:8580-8586
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