Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments

被引:139
作者
Chirico, R. [1 ,2 ]
DeCarlo, P. F. [1 ]
Heringa, M. F. [1 ]
Tritscher, T. [1 ]
Richter, R. [1 ]
Prevot, A. S. H. [1 ]
Dommen, J. [1 ]
Weingartner, E. [1 ]
Wehrle, G. [1 ]
Gysel, M. [1 ]
Laborde, M. [1 ]
Baltensperger, U. [1 ]
机构
[1] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
[2] FIS LAS, Italian Natl Agcy New Technol Energy & Sustainabl, I-00044 Frascati, Italy
基金
瑞士国家科学基金会; 美国国家科学基金会;
关键词
AERODYNAMIC DIAMETER MEASUREMENTS; LASER-INDUCED INCANDESCENCE; MASS-SPECTROMETER; BLACK CARBON; HIGH-RESOLUTION; DENSITY CHARACTERIZATION; PHOTOCHEMICAL OXIDATION; PARTICULATE-EMISSIONS; PARTICLE MORPHOLOGY; COMBINED MOBILITY;
D O I
10.5194/acp-10-11545-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Diesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the third vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC <0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging similar to 80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23-0.56 g/kg fuel burned. In presence of both a DOC and a DPF, only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.10 to 0.19. Five hours of oxidation led to a more oxidized OA with an O/C range of 0.21 to 0.37.
引用
收藏
页码:11545 / 11563
页数:19
相关论文
共 58 条
  • [1] *ACEA, 2008, EU EC REP
  • [2] O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry
    Aiken, Allison C.
    Decarlo, Peter F.
    Kroll, Jesse H.
    Worsnop, Douglas R.
    Huffman, J. Alex
    Docherty, Kenneth S.
    Ulbrich, Ingrid M.
    Mohr, Claudia
    Kimmel, Joel R.
    Sueper, Donna
    Sun, Yele
    Zhang, Qi
    Trimborn, Achim
    Northway, Megan
    Ziemann, Paul J.
    Canagaratna, Manjula R.
    Onasch, Timothy B.
    Alfarra, M. Rami
    Prevot, Andre S. H.
    Dommen, Josef
    Duplissy, Jonathan
    Metzger, Axel
    Baltensperger, Urs
    Jimenez, Jose L.
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) : 4478 - 4485
  • [3] Elemental analysis of organic species with electron ionization high-resolution mass spectrometry
    Aiken, Allison. C.
    DeCarlo, Peter F.
    Jimenez, Jose L.
    [J]. ANALYTICAL CHEMISTRY, 2007, 79 (21) : 8350 - 8358
  • [4] Characterization of urban and rural organic particulate in the lower Fraser valley using two aerodyne aerosol mass spectrometers
    Alfarra, MR
    Coe, H
    Allan, JD
    Bower, KN
    Boudries, H
    Canagaratna, MR
    Jimenez, JL
    Jayne, JT
    Garforth, AA
    Li, SM
    Worsnop, DR
    [J]. ATMOSPHERIC ENVIRONMENT, 2004, 38 (34) : 5745 - 5758
  • [5] A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data
    Allan, JD
    Delia, AE
    Coe, H
    Bower, KN
    Alfarra, MR
    Jimenez, JL
    Middlebrook, AM
    Drewnick, F
    Onasch, TB
    Canagaratna, MR
    Jayne, JT
    Worsnop, DR
    [J]. JOURNAL OF AEROSOL SCIENCE, 2004, 35 (07) : 909 - 922
  • [6] Deactivation of diesel oxidation catalysts: Vehicle- and synthetic aging correlations
    Andersson, Jonas
    Antonsson, Matilda
    Eurenius, Lisa
    Olsson, Eva
    Skoglundh, Magnus
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 72 (1-2) : 71 - 81
  • [7] [Anonymous], 2002, HLTH ASS DOC DIES EN
  • [8] Atmospheric degradation of volatile organic compounds
    Atkinson, R
    Arey, J
    [J]. CHEMICAL REVIEWS, 2003, 103 (12) : 4605 - 4638
  • [9] Chemical analysis of atmospheric aerosols
    Baltensperger, Urs
    Prevot, Andre S. H.
    [J]. ANALYTICAL AND BIOANALYTICAL CHEMISTRY, 2008, 390 (01) : 277 - 280
  • [10] Bostock David., 2006, Space, Time, Matter, and Form: Essays on Aristotle's Physics, P1