Molecular composition of fresh and aged secondary organic aerosol from a mixture of biogenic volatile compounds: a high-resolution mass spectrometry study

作者: I. Kourtchev , J.-F. Doussin , C. Giorio , B. Mahon , E. M. Wilson

DOI: 10.5194/ACP-15-5683-2015

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摘要: Abstract. Field observations over the past decade indicate that a significant fraction of organic aerosol in remote areas may contain highly oxidized molecules. Aerosol processing or further oxidation (aging) has been suggested to be responsible for their formation through heterogeneous reaction with oxidants and multigenerational vapours by OH radicals. In this study we investigated influence several aging processes on molecular composition secondary aerosols (SOA) using direct infusion liquid chromatography high-resolution mass spectrometry. SOA was formed simulation chamber experiments from ozonolysis mixture four biogenic volatile compounds (BVOC): α-pinene, β-pinene, Δ3-carene isoprene. The subsequently aged under three different sets conditions: dark presence residual ozone, UV irradiation radicals, light only. Among all studied conditions, only radical-initiated found showed an increase carbon state (OSC) elemental O / C ratios components. None produced observable effect oligomers BVOC mixture, which were equally abundant both "fresh" "aged" SOA. Additional α-pinene as sole precursor demonstrated are important group processes; however, completely set is these two regimes. OH-initiated had significantly higher overall OSC compared pure confirming radical more likely occurrence species ambient

参考文章(64)
Jianzhen Yu, David R. Cocker III, Robert J. Griffin, Richard C. Flagan, John H. Seinfeld, Gas-phase ozone oxidation of monoterpenes: Gaseous and particulate products Journal of Atmospheric Chemistry. ,vol. 34, pp. 207- 258 ,(1999) , 10.1023/A:1006254930583
R. Atkinson, D. L. Baulch, R. A. Cox, R. F. Hampson, J. A. Kerr, M. J. Rossi, J. Troe, Evaluated Kinetic, Photochemical and Heterogeneous Data for Atmospheric Chemistry: Supplement V.   IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry Journal of Physical and Chemical Reference Data. ,vol. 26, pp. 521- 1011 ,(1997) , 10.1063/1.556011
R. A. Cox, R. F. Hampson, J. A. Kerr, M. J. Rossi, J. Troe, R. Atkinson, D. L. Baulch, Evaluated Kinetic and Photochemical Data for Atmospheric Chemistry: Supplement VI. IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry Journal of Physical and Chemical Reference Data. ,vol. 26, pp. 1329- 1499 ,(1997) , 10.1063/1.556010
H. Aaltonen, J. Pumpanen, M. Pihlatie, H. Hakola, H. Hellén, L. Kulmala, T. Vesala, J. Bäck, Boreal pine forest floor biogenic volatile organic compound emissions peak in early summer and autumn Agricultural and Forest Meteorology. ,vol. 151, pp. 682- 691 ,(2011) , 10.1016/J.AGRFORMET.2010.12.010
A. L. Robinson, N. M. Donahue, M. K. Shrivastava, E. A. Weitkamp, A. M. Sage, A. P. Grieshop, T. E. Lane, J. R. Pierce, S. N. Pandis, Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging Science. ,vol. 315, pp. 1259- 1262 ,(2007) , 10.1126/SCIENCE.1133061
Rafal Szmigielski, Jason D. Surratt, Yadian Gómez-González, Pieter Van der Veken, Ivan Kourtchev, Reinhilde Vermeylen, Frank Blockhuys, Mohammed Jaoui, Tadeusz E. Kleindienst, Michael Lewandowski, John H. Offenberg, Edward O. Edney, John H. Seinfeld, Willy Maenhaut, Magda Claeys, 3‐methyl‐1,2,3‐butanetricarboxylic acid: An atmospheric tracer for terpene secondary organic aerosol Geophysical Research Letters. ,vol. 34, ,(2007) , 10.1029/2007GL031338
Ivan Kourtchev, Stephen Fuller, Juho Aalto, Taina M. Ruuskanen, Matthew W. McLeod, Willy Maenhaut, Rod Jones, Markku Kulmala, Markus Kalberer, Molecular composition of boreal forest aerosol from Hyytiälä, Finland, using ultrahigh resolution mass spectrometry. Environmental Science & Technology. ,vol. 47, pp. 4069- 4079 ,(2013) , 10.1021/ES3051636
J. Wang, J. F. Doussin, S. Perrier, E. Perraudin, Y. Katrib, E. Pangui, B. Picquet-Varrault, Design of a new multi-phase experimental simulation chamber for atmospheric photosmog, aerosol and cloud chemistry research Atmospheric Measurement Techniques. ,vol. 4, pp. 2465- 2494 ,(2011) , 10.5194/AMT-4-2465-2011
Marianne Glasius, Maria Lahaniati, Aggelos Calogirou, Dario Di Bella, Niels R. Jensen, Jens Hjorth, Dimitrios Kotzias, Bo R. Larsen, Carboxylic Acids in Secondary Aerosols from Oxidation of Cyclic Monoterpenes by Ozone Environmental Science & Technology. ,vol. 34, pp. 1001- 1010 ,(2000) , 10.1021/ES990445R
Albert A. Presto, Neil M. Donahue, Ozonolysis Fragment Quenching by Nitrate Formation: The Pressure Dependence of Prompt OH Radical Formation Journal of Physical Chemistry A. ,vol. 108, pp. 9096- 9104 ,(2004) , 10.1021/JP047162S