Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City

被引:71
作者
Moffet, R. C. [1 ]
Henn, T. R. [1 ,2 ]
Tivanski, A. V. [1 ]
Hopkins, R. J. [1 ]
Desyaterik, Y. [3 ]
Kilcoyne, A. L. D. [1 ]
Tyliszczak, T. [1 ]
Fast, J. [4 ]
Barnard, J. [4 ]
Shutthanandan, V. [3 ]
Cliff, S. S. [5 ]
Perry, K. D. [6 ]
Laskin, A. [3 ]
Gilles, M. K. [1 ]
机构
[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA
[2] Univ Wurzburg, Dept Phys, D-97074 Wurzburg, Germany
[3] Pacific NW Natl Lab, WR Wiley Environm Mol Sci Lab, Richland, WA 99352 USA
[4] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA
[5] Univ Calif Davis, Dept Appl Sci, Davis, CA 95616 USA
[6] Univ Utah, Dept Meteorol, Salt Lake City, UT 84112 USA
关键词
MILAGRO FIELD CAMPAIGN; X-RAY-MICROANALYSIS; SOURCE APPORTIONMENT; MASS-SPECTROMETRY; ORGANIC AEROSOLS; BLACK CARBON; ATMOSPHERIC PARTICLES; INDIVIDUAL PARTICLES; MCMA-2003; CAMPAIGN; METROPOLITAN-AREA;
D O I
10.5194/acp-10-961-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study was part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in Mexico City metropolitan area during spring 2006. The physical and chemical transformations of particles aged in the outflow from Mexico City were investigated for the transport event of 22 March 2006. A detailed chemical analysis of individual particles was performed using a combination of complementary microscopy and micro-spectroscopy techniques. The applied techniques included scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure spectroscopy (NEXAFS) and computer controlled scanning electron microscopy with an energy dispersive X-ray analyzer (CCSEM/EDX). As the aerosol plume evolves from the city center, the organic mass per particle increases and the fraction of carbon-carbon double bonds (associated with elemental carbon) decreases. Organic functional groups enhanced with particle age include: carboxylic acids, alkyl groups, and oxygen bonded alkyl groups. At the city center (T0) the most prevalent aerosol type contained inorganic species (composed of sulfur, nitrogen, oxygen, and potassium) coated with organic material. At the T1 and T2 sites, located northeast of T0 (similar to 29 km and similar to 65 km, respectively), the fraction of homogenously mixed organic particles increased in both size and number. These observations illustrate the evolution of the physical mixing state and organic bonding in individual particles in a photochemically active environment.
引用
收藏
页码:961 / 976
页数:16
相关论文
共 73 条
[11]   Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer [J].
Canagaratna, M. R. ;
Jayne, J. T. ;
Jimenez, J. L. ;
Allan, J. D. ;
Alfarra, M. R. ;
Zhang, Q. ;
Onasch, T. B. ;
Drewnick, F. ;
Coe, H. ;
Middlebrook, A. ;
Delia, A. ;
Williams, L. R. ;
Trimborn, A. M. ;
Northway, M. J. ;
DeCarlo, P. F. ;
Kolb, C. E. ;
Davidovits, P. ;
Worsnop, D. R. .
MASS SPECTROMETRY REVIEWS, 2007, 26 (02) :185-222
[12]   Evidence for liquid-like and nonideal behavior of a mixture of organic aerosol components [J].
Cappa, Christopher D. ;
Lovejoy, Edward R. ;
Ravishankara, A. R. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (48) :18687-18691
[13]   Basin-scale wind transport during the MILAGRO field campaign and comparison to climatology using cluster analysis [J].
de Foy, B. ;
Fast, J. D. ;
Paech, S. J. ;
Phillips, D. ;
Walters, J. T. ;
Coulter, R. L. ;
Martin, T. J. ;
Pekour, M. S. ;
Shaw, W. J. ;
Kastendeuch, P. P. ;
Marley, N. A. ;
Retama, A. ;
Molina, L. T. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (05) :1209-1224
[14]   Applications of lagrangian dispersion modeling to the analysis of changes in the specific absorption of elemental carbon [J].
Doran, J. C. ;
Fast, J. D. ;
Barnard, J. C. ;
Laskin, A. ;
Desyaterik, Y. ;
Gilles, M. K. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (05) :1377-1389
[15]   The T1-T2 study: evolution of aerosol properties downwind of Mexico City [J].
Doran, J. C. ;
Barnard, J. C. ;
Arnott, W. P. ;
Cary, R. ;
Coulter, R. ;
Fast, J. D. ;
Kassianov, E. I. ;
Kleinman, L. ;
Laulainen, N. S. ;
Martin, T. ;
Paredes-Miranda, G. ;
Pekour, M. S. ;
Shaw, W. J. ;
Smith, D. F. ;
Springston, S. R. ;
Yu, X. -Y. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2007, 7 (06) :1585-1598
[16]  
Doran JC, 1998, B AM METEOROL SOC, V79, P2497, DOI 10.1175/1520-0477(1998)079<2497:TIABLE>2.0.CO
[17]  
2
[18]   Radiation damage in the TEM and SEM [J].
Egerton, RF ;
Li, P ;
Malac, M .
MICRON, 2004, 35 (06) :399-409
[19]   Evaluating simulated primary anthropogenic and biomass burning organic aerosols during MILAGRO: implications for assessing treatments of secondary organic aerosols [J].
Fast, J. ;
Aiken, A. C. ;
Allan, J. ;
Alexander, L. ;
Campos, T. ;
Canagaratna, M. R. ;
Chapman, E. ;
DeCarlo, P. F. ;
de Foy, B. ;
Gaffney, J. ;
de Gouw, J. ;
Doran, J. C. ;
Emmons, L. ;
Hodzic, A. ;
Herndon, S. C. ;
Huey, G. ;
Jayne, J. T. ;
Jimenez, J. L. ;
Kleinman, L. ;
Kuster, W. ;
Marley, N. ;
Russell, L. ;
Ochoa, C. ;
Onasch, T. B. ;
Pekour, M. ;
Song, C. ;
Ulbrich, I. M. ;
Warneke, C. ;
Welsh-Bon, D. ;
Wiedinmyer, C. ;
Worsnop, D. R. ;
Yu, X. -Y. ;
Zaveri, R. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (16) :6191-6215
[20]  
FAST JD, 2006, 7 WRF US WORKSH