On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City

被引:59
作者
Hennigan, C. J. [1 ]
Sullivan, A. P. [2 ]
Fountoukis, C. I. [3 ]
Nenes, A. [2 ,3 ]
Hecobian, A. [2 ]
Vargas, O. [2 ]
Peltier, R. E. [2 ]
Hanks, A. T. Case [2 ]
Huey, L. G. [2 ]
Lefer, B. L. [4 ]
Russell, A. G. [1 ]
Weber, R. J. [2 ]
机构
[1] Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA
[2] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[3] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[4] Univ Houston, Dept Geosci, Houston, TX 77204 USA
关键词
D O I
10.5194/acp-8-3761-2008
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Measurements of atmospheric gases and fine particle chemistry were made in the Mexico City Metropolitan Area (MCMA) at a site similar to 30 km down wind of the city center. Ammonium nitrate (NH4NO3) dominated the inorganic aerosol fraction and showed a distinct diurnal signature characterized by rapid morning production and a rapid mid-day concentration decrease. Between the hours of 08:00-12:45, particulate water-soluble organic carbon (WSOC) concentrations increased and decreased in a manner consistent with that of NO3-, and the two were highly correlated (R-2=0.88) during this time. A box model was used to analyze these behaviors and showed that, for both NO3-, and WSOC, the concentration increase was caused primarily (similar to 75-85%) by secondary formation, with a smaller contribution (similar to 15-25%) from the entrainment of air from the free troposphere. For NO3-, a majority (similar to 60%) of the midday concentration decrease was caused by dilution from boundary layer expansion, though a significant fraction (similar to 40%) of the NO3- loss was due to particle evaporation. The WSOC concentration decrease was due largely to dilution (similar to 75%), but volatilization did have a meaningful impact (similar to 25%) on the decrease, as well. The results provide an estimate of ambient SOA evaporation losses and suggest that a significant fraction (similar to 35%) of the fresh MCMA secondary organic aerosol (SOA) measured at the surface volatilized.
引用
收藏
页码:3761 / 3768
页数:8
相关论文
共 32 条
[1]   Aerosol volatility measurement using an improved thermodenuder: Application to secondary organic aerosol [J].
An, Woo Jin ;
Pathak, Ravi K. ;
Lee, Byong-Hyoek ;
Pandis, Spyros N. .
JOURNAL OF AEROSOL SCIENCE, 2007, 38 (03) :305-314
[2]   Measurement of gas-phase hydroperoxides by chemical ionization mass spectrometry [J].
Crounse, John D. ;
McKinney, Karena A. ;
Kwan, Alan J. ;
Wennberg, Paul O. .
ANALYTICAL CHEMISTRY, 2006, 78 (19) :6726-6732
[3]   Volatile organic compounds composition of merged and aged forest fire plumes from Alaska and western Canada [J].
de Gouw, J. A. ;
Warneke, C. ;
Stohl, A. ;
Wollny, A. G. ;
Brock, C. A. ;
Cooper, O. R. ;
Holloway, J. S. ;
Trainer, M. ;
Fehsenfeld, F. C. ;
Atlas, E. L. ;
Donnelly, S. G. ;
Stroud, V. ;
Lueb, A. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2006, 111 (D10)
[4]   Semi-volatile secondary organic aerosol in urban atmospheres: meeting a measurement challenge [J].
Eatough, DJ ;
Long, RW ;
Modey, WK ;
Eatough, NL .
ATMOSPHERIC ENVIRONMENT, 2003, 37 (9-10) :1277-1292
[5]   ISORROPIA II:: a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-Nh4+-Na+-SO42--NO3--Cl--H2O aerosols [J].
Fountoukis, C. ;
Nenes, A. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2007, 7 (17) :4639-4659
[6]  
FOUNTOUKIS C, 2007, ATMOS CHEM PHYS DISC, V7, P9203, DOI DOI 10.5194/ACPD-7-9203-2007
[7]   Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible? [J].
Grieshop, Andrew P. ;
Donahue, Neil M. ;
Robinson, Allen L. .
GEOPHYSICAL RESEARCH LETTERS, 2007, 34 (14)
[8]   Global secondary organic aerosol from isoprene oxidation [J].
Henze, Daven K. ;
Seinfeld, John H. .
GEOPHYSICAL RESEARCH LETTERS, 2006, 33 (09)
[9]   Identification of polymers as major components of atmospheric organic aerosols [J].
Kalberer, M ;
Paulsen, D ;
Sax, M ;
Steinbacher, M ;
Dommen, J ;
Prevot, ASH ;
Fisseha, R ;
Weingartner, E ;
Frankevich, V ;
Zenobi, R ;
Baltensperger, U .
SCIENCE, 2004, 303 (5664) :1659-1662
[10]   Organic aerosol and global climate modelling: a review [J].
Kanakidou, M ;
Seinfeld, JH ;
Pandis, SN ;
Barnes, I ;
Dentener, FJ ;
Facchini, MC ;
Van Dingenen, R ;
Ervens, B ;
Nenes, A ;
Nielsen, CJ ;
Swietlicki, E ;
Putaud, JP ;
Balkanski, Y ;
Fuzzi, S ;
Horth, J ;
Moortgat, GK ;
Winterhalter, R ;
Myhre, CEL ;
Tsigaridis, K ;
Vignati, E ;
Stephanou, EG ;
Wilson, J .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2005, 5 :1053-1123