成都市冬季挥发性有机物污染特征及来源研究
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摘要
利用挥发性有机物在线监测仪(GC-FID/MS)在成都市市区开展为期一个月的挥发性有机物监测,分析了VOCs浓度水平、组分构成、日变化规律,并分别利用PMF模型和排放清单法对VOCs的来源进行解析研究。结果表明,监测期间,VOCs小时平均浓度为7610~(-9),最高浓度为26210~(-9),最低浓度为14.810~(-9);监测物种类别中烷烃类占VOCs总体积浓度为38%,炔烃为17%,芳香烃为15%,烯烃为13%,卤代烃为9%,含氧(氮)类化合物为8%,浓度前十的物种分别为乙烷、乙炔、乙烯、丙烷、甲苯、己醛、二氯甲烷、苯、正丁烷和异戊烷,占总浓度的70%以上。烷烃、炔烃、烯烃、芳香烃在8点～10点间均出现浓度峰值,芳香烃、卤代烃以及含氧(氮)化合物浓度最高值出现在凌晨2点～5点;最低浓度则均出现在下午17点左右。基于PMF的方法,VOCs的来源解析结果为工业源贡献32%,机动车贡献26%,生物质燃烧贡献22%,溶剂源贡献7%,油气挥发贡献6%,本底混合源贡献7%;基于排放清单法,2015年成都市VOCs年排放量为36.9万t,工艺过程源、溶剂使用源、移动源分别贡献32%、32%、30%。
99 species of VOCs were monitored for one month by VOCs online monitor in Chengdu City,in December, 2015. The hourly average concentration of the total VOCs was 76×10~(-9), the highest concentration was 262×10~(-9), while the lowest concentration was 14.8×10~(-9). Alkane, alkyne, aromatic, alkene, and halohydrocarbon accounted for 38%,17%,15%,13%,and 9% of the total VOCs concentration, respectively, while compounds containing oxygen(nitrogen) accounted for 8%. The top ten species were ethane, acetylene, ethylene, propane, toluene, hexanal, methylene chloride, benzene, n-butane and isopentane, contributing more than 70% of the total concentration. Peak concentration of Alkanes, alkene, alkynes and aromatics appeared between 8～10 am, for the other species categories, the highest concentration occurred in the early morning 2～5 am. The lowest concentration for all the VOCs species appeared at 5 pm. The PMF model and emission inventory method was used for source apportionment of VOCs in Chengdu, 6 categories of emission sources were determined. The industry source, vehicle source, biomass burning, solvent using, oil evaporation and the background source contributing 32%, 26%,22%,7%, 6%, and 7% of the VOCs, respectively, however, the result of the emission inventory showed industry source, vehicle source, solvent using contributing 32%, 30%,32% of the total annual emission of organic compounds in Chengdu in 2015, which was 36.9×10~4 tons.
99 species of VOCs were monitored for one month by VOCs online monitor in Chengdu City,in December, 2015. The hourly average concentration of the total VOCs was 76×10~(-9), the highest concentration was 262×10~(-9), while the lowest concentration was 14.8×10~(-9). Alkane, alkyne, aromatic, alkene, and halohydrocarbon accounted for 38%,17%,15%,13%,and 9% of the total VOCs concentration, respectively, while compounds containing oxygen(nitrogen) accounted for 8%. The top ten species were ethane, acetylene, ethylene, propane, toluene, hexanal, methylene chloride, benzene, n-butane and isopentane, contributing more than 70% of the total concentration. Peak concentration of Alkanes, alkene, alkynes and aromatics appeared between 8～10 am, for the other species categories, the highest concentration occurred in the early morning 2～5 am. The lowest concentration for all the VOCs species appeared at 5 pm. The PMF model and emission inventory method was used for source apportionment of VOCs in Chengdu, 6 categories of emission sources were determined. The industry source, vehicle source, biomass burning, solvent using, oil evaporation and the background source contributing 32%, 26%,22%,7%, 6%, and 7% of the VOCs, respectively, however, the result of the emission inventory showed industry source, vehicle source, solvent using contributing 32%, 30%,32% of the total annual emission of organic compounds in Chengdu in 2015, which was 36.9×10~4 tons.
引文
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[31] 韩博,吴建会,王凤炜,等.典型工业恶臭源恶臭排放特征研究[J].中国环境科学,2013,33(3):416-422.
[32] 崔彤,程婧晨,何万清,等.北京市典型餐饮企业 VOCs 排放特征研究[J].环境科学,2015,(5):1523-1529.
[2] 四川省环境保护厅.四川省环境状况公报[R].四川,2016.
[3] 钱骏,廖瑞雪,邓利群,等.成都市大气中O3污染水平及来源分析[J].四川环境,2011,30(3):20-23.
[4] 环保部,“十三五”挥发性有机物污染防治工作方案[R].北京,2017.
[5] Wang M,Zeng L,Lu S,et al.Development and validation of a cryogen-free automatic gas chromatograph system (GC-MS/FID) for online measurements of volatile organic compounds[J].Analytical Methods,2014,6(23):9424-9434.
[6] Li J,Xie S D,Zeng L M,et al.Characterization of ambient volatile organic compounds and their sources in Beijing,before,during,and after Asia-Pacific Economic Cooperation China 2014[J].Atmospheric Chemistry & Physics,2015,15(8):12453-12490.
[7] Salameh T,Sauvage S,Afif C,et al.Source apportionment vs.emission inventories of non-methane hydrocarbons (NMHC) in an urban area of the Middle East:local and global perspectives[J].Atmospheric Chemistry & Physics,2016,15(19):26795-26837.
[8] 张玉欣,安俊琳,王俊秀,等.南京工业区挥发性有机物来源解析及其对臭氧贡献评估[J].环境科学,2018,(2) :502-510.
[9] 高蒙,安俊琳,杭一纤,等.PMF和PCA/APCS模型对南京北郊大气VOCs源解析对比研究[J].气象与环境学报,2014,(1):43-50.
[10] U.S.EPA,EPA positive matrix factorization (PMF) 5.0 fundamentals and user guide[EB/OL].https://www.epa.gov/air-research/epa-positive-matrix-factorization-50-fundamentals-and-user-guide,2014.
[11] Yuan B,Shao M,Gouw J D,et al.Volatile organic compounds (VOCs) in urban air:How chemistry affects the interpretation of positive matrix factorization (PMF) analysis[J].Journal of Geophysical Research Atmospheres,2012,117(D24):24302.
[12] 四川省环境保护科学研究院.四川省大气挥发性有机物排放调查系统[EB/OL].http://www.scaes.cn/kq/,2017.
[13] 四川省环境保护科学研究院.大气污染源排放清单数字化平台[EB/OL].http://www.scaes.cn/kq/,2017.
[14] 环境保护部.大气挥发性有机物源排放清单编制技术指南(试行)[R],2014.
[15] 尹元畅,蒋燕,王波,等.成都餐饮源PM2.5及VOCs排放因子的探索[J].环境监测管理与技术,2015,27(5):63-67.
[16] 莫梓伟,邵敏,陆思华.中国挥发性有机物(VOCs)排放源成分谱研究进展[J].环境科学学报,2014,34(9):2179-2189.
[17] Li L,Chen Y,Zeng L,et al.Biomass burning contribution to ambient volatile organic compounds (VOCs) in the Chengdu–Chongqing Region (CCR),China[J].Atmospheric Environment,2014,99:403-410.
[18] Zou Y,Deng X J,Zhu D,et al.Characteristics of 1 year of observational data of VOCs,NOx and O3 at a suburban site in Guangzhou,China[J].Atmospheric Chemistry & Physics,2015,15(12):6625-6636.
[19] 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,2016,117(117):304-315.
[20] 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,(1):11-17.
[21] 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.
[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.
[23] Barletta B,Meinardi S,Rowland F S,et al.Volatile organic compounds in 43 Chinese cities[J].Atmospheric Environment,2005,39(32):5979-5990.
[24] Liu Y,Fu S L,Lu S,et al.Source profiles of volatile organic compounds (VOCs) measured in China:Part I[J].Atmospheric Environment,2008,42(25):6247-6260
[25] De Gouw J A,Warneke C,Parrish D D,et al.Emission sources and ocean uptake of acetonitrile (CH3CN) in the atmosphere[J].Journal of Geophysical Research Atmospheres,2003,108(D11):4329.
[26] 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
[27] 王琛.广州大气中挥发性卤代烃的时空分布特征与来源分析研究[D].广州:暨南大学,2010.
[28] 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.
[29] Yuan B,Shao M,Lu S H,Wang B.Source profiles of volatile organic compounds associated with solvent use in Beijing[J].Atmospheric Environment,2010,44:1919-1926.
[30] Mo Z,Shao M,Lu S.Compilation of a source profile database for hydrocarbon and OVOC emissions in China[J].Atmospheric Environment,2016,143:209-217.
[31] 韩博,吴建会,王凤炜,等.典型工业恶臭源恶臭排放特征研究[J].中国环境科学,2013,33(3):416-422.
[32] 崔彤,程婧晨,何万清,等.北京市典型餐饮企业 VOCs 排放特征研究[J].环境科学,2015,(5):1523-1529.