Emission ratios of anthropogenic volatile organic compounds in northern mid-latitude megacities: Observations versus emission inventories in Los Angeles and Paris

被引:205
作者
Borbon, Agnes [1 ,2 ,3 ,4 ]
Gilman, J. B. [3 ,4 ]
Kuster, W. C. [3 ,4 ]
Grand, N. [1 ,2 ]
Chevaillier, S. [1 ,2 ]
Colomb, A. [1 ,2 ]
Dolgorouky, C. [5 ]
Gros, V. [5 ]
Lopez, M. [5 ]
Sarda-Esteve, R. [5 ]
Holloway, J. [3 ,4 ]
Stutz, J. [6 ]
Petetin, H. [1 ,2 ]
McKeen, S. [3 ,4 ]
Beekmann, M. [1 ,2 ]
Warneke, C. [3 ,4 ]
Parrish, D. D. [4 ]
de Gouw, J. A. [3 ,4 ]
机构
[1] UPEC, LISA, IPSL, UMR CNRS 7583, F-94010 Creteil, France
[2] UPD, F-94010 Creteil, France
[3] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[4] NOAA, Earth Syst Res Lab, Boulder, CO USA
[5] Univ Versailles St Quentin En Yvelines, Lab Sci Climat & Environm, CEA, CNRS, Gif Sur Yvette, France
[6] Univ Calif Los Angeles, Dept Atmospher Sci, Los Angeles, CA 90024 USA
关键词
NONMETHANE HYDROCARBON CHARACTERIZATION; RECEPTOR-ORIENTED METHODS; FLUX MEASUREMENTS; AEROSOL FORMATION; OZONE FORMATION; URBAN AIR; VOC; HOUSTON; CO; SEMIVOLATILE;
D O I
10.1002/jgrd.50059
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
Ground-based and airborne volatile organic compound (VOC) measurements in Los Angeles, California, and Paris, France, during the Research at the Nexus of Air Quality and Climate Change (CalNex) and Megacities: Emissions, Urban, Regional and Global Atmospheric Pollution and Climate Effects, and Integrated Tools for Assessment and Mitigation (MEGAPOLI) campaigns, respectively, are used to examine the spatial variability of the composition of anthropogenic VOC urban emissions and to evaluate regional emission inventories. Two independent methods that take into account the effect of chemistry were used to determine the emission ratios of anthropogenic VOCs (including anthropogenic isoprene and oxygenated VOCs) over carbon monoxide (CO) and acetylene. Emission ratios from both methods agree within +/- 20%, showing the reliability of our approach. Emission ratios for alkenes, alkanes, and benzene are fairly similar between Los Angeles and Paris, whereas the emission ratios for C7-C9 aromatics in Paris are higher than in Los Angeles and other French and European Union urban areas by a factor of 2-3. The results suggest that the emissions of gasoline-powered vehicles still dominate the hydrocarbon distribution in northern mid-latitude urban areas, which disagrees with emission inventories. However, regional characteristics like the gasoline composition could affect the composition of hydrocarbon emissions. The observed emission ratios show large discrepancies by a factor of 2-4 (alkanes and oxygenated VOC) with the ones derived from four reference emission databases. A bias in CO emissions was also evident for both megacities. Nevertheless, the difference between measurements and inventory in terms of the overall OH reactivity is, in general, lower than 40%, and the potential to form secondary organic aerosols (SOA) agrees within 30% when considering volatile organic emissions as the main SOA precursors. Citation: Borbon, A., et al. (2013), Emission ratios of anthropogenic volatile organic compounds in northern mid-latitude megacities: Observations versus emission inventories in Los Angeles and Paris, J. Geophys. Res. Atmos., 118, 2041-2057, doi: 10.1002/jgrd.50059.
引用
收藏
页码:2041 / 2057
页数:17
相关论文
共 65 条
[1]   Chemical Characterization of Emissions from Modern Two-Stroke Mopeds Complying with Legislative Regulation in Europe (EURO-2) [J].
Adam, T. ;
Farfaletti, A. ;
Montero, L. ;
Martini, G. ;
Manfredi, U. ;
Larsen, B. ;
De Santi, G. ;
Krasenbrink, A. ;
Astorga, C. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (01) :505-512
[2]   Impact of nitrous acid photolysis on the total hydroxyl radical budget during the Limitation of Oxidant Production/Pianura Padana Produzione di Ozono study in Milan [J].
Alicke, B ;
Platt, U ;
Stutz, J .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2002, 107 (D22)
[3]   Contributions from transport, solid fuel burning and cooking to primary organic aerosols in two UK cities [J].
Allan, J. D. ;
Williams, P. I. ;
Morgan, W. T. ;
Martin, C. L. ;
Flynn, M. J. ;
Lee, J. ;
Nemitz, E. ;
Phillips, G. J. ;
Gallagher, M. W. ;
Coe, H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (02) :647-668
[4]   Nighttime nitrate radical chemistry at Appledore island, Maine during the 2004 international consortium for atmospheric research on transport and transformation [J].
Ambrose, J. L. ;
Mao, H. ;
Mayne, H. R. ;
Stutz, J. ;
Talbot, R. ;
Sive, B. C. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D21)
[5]   Atmospheric degradation of volatile organic compounds [J].
Atkinson, R ;
Arey, J .
CHEMICAL REVIEWS, 2003, 103 (12) :4605-4638
[6]   An automated monitoring system for VOC ozone precursors in ambient air:: development, implementation and data analysis [J].
Badol, C ;
Borbon, A ;
Locoge, N ;
Léonardis, T ;
Galloo, JC .
ANALYTICAL AND BIOANALYTICAL CHEMISTRY, 2004, 378 (07) :1815-1827
[7]   Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass [J].
Bahreini, R. ;
Middlebrook, A. M. ;
de Gouw, J. A. ;
Warneke, C. ;
Trainer, M. ;
Brock, C. A. ;
Stark, H. ;
Brown, S. S. ;
Dube, W. P. ;
Gilman, J. B. ;
Hall, K. ;
Holloway, J. S. ;
Kuster, W. C. ;
Perring, A. E. ;
Prevot, A. S. H. ;
Schwarz, J. P. ;
Spackman, J. R. ;
Szidat, S. ;
Wagner, N. L. ;
Weber, R. J. ;
Zotter, P. ;
Parrish, D. D. .
GEOPHYSICAL RESEARCH LETTERS, 2012, 39
[8]   Measurements of nonmethane hydrocarbons in 28 United States cities [J].
Baker, Angela K. ;
Beyersdorf, Andreas J. ;
Doezema, Lambert A. ;
Katzenstein, Aaron ;
Meinardi, Simone ;
Simpson, Isobel J. ;
Blake, Donald R. ;
Rowland, F. Sherwood .
ATMOSPHERIC ENVIRONMENT, 2008, 42 (01) :170-182
[9]   Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution [J].
Bon, D. M. ;
Ulbrich, I. M. ;
de Gouw, J. A. ;
Warneke, C. ;
Kuster, W. C. ;
Alexander, M. L. ;
Baker, A. ;
Beyersdorf, A. J. ;
Blake, D. ;
Fall, R. ;
Jimenez, J. L. ;
Herndon, S. C. ;
Huey, L. G. ;
Knighton, W. B. ;
Ortega, J. ;
Springston, S. ;
Vargas, O. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (06) :2399-2421
[10]   An investigation into the traffic-related fraction of isoprene at an urban location [J].
Borbon, A ;
Fontaine, H ;
Veillerot, M ;
Locoge, N ;
Galloo, JC ;
Guillermo, R .
ATMOSPHERIC ENVIRONMENT, 2001, 35 (22) :3749-3760