Aqueous OH oxidation of ambient organic aerosol and cloud water organics: Formation of highly oxidized products

被引:95
作者
Lee, Alex K. Y. [1 ]
Herckes, P. [2 ]
Leaitch, W. R. [3 ]
Macdonald, A. M. [3 ]
Abbatt, J. P. D. [1 ]
机构
[1] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada
[2] Arizona State Univ, Dept Chem & Biochem, Tempe, AZ 85287 USA
[3] Environm Canada, Sci & Technol Branch, Toronto, ON M3H 5T4, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
MASS-SPECTROMETER; CHEMISTRY; GLYOXAL; PARTICLES; EVOLUTION; SPECTRA; PHASE;
D O I
10.1029/2011GL047439
中图分类号
P [天文学、地球科学];
学科分类号
07 ;
摘要
Aqueous chemistry can play a vital role in secondary organic aerosol (SOA) formation and aging. A novel analytical approach that allows for simultaneous photo-oxidation and atomization of reacting bulk solutions coupled to an aerosol mass spectrometer (AMS) investigates aqueous OH oxidation of ambient biogenic SOA, cloud water from a biogenic environment, glyoxal, and mixtures of glyoxal with alpha-pinene SOA components. This is the first study of aqueous oxidative aging of ambient SOA and cloud water organics. Starting with an AMS-based observational framework, we show that aqueous oxidation of biogenic SOA in the presence of glyoxal can better represent observed atmospheric aging than when glyoxal is absent. Oxidation of glyoxal alongside semi-volatile SOA components leads to the production of highly oxidized SOA. Citation: Lee, A. K. Y., P. Herckes, W. R. Leaitch, A. M. Macdonald, and J. P. D. Abbatt (2011), Aqueous OH oxidation of ambient organic aerosol and cloud water organics: Formation of highly oxidized products, Geophys. Res. Lett., 38, L11805, doi: 10.1029/2011GL047439.
引用
收藏
页数:5
相关论文
共 23 条
[1]   Measurements of secondary organic aerosol from oxidation of cycloalkenes, terpenes, and m-xylene using an Aerodyne aerosol mass spectrometer [J].
Bahreini, R ;
Keywood, MD ;
Ng, NL ;
Varutbangkul, V ;
Gao, S ;
Flagan, RC ;
Seinfeld, JH ;
Worsnop, DR ;
Jimenez, JL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (15) :5674-5688
[2]   CMAQ Model Performance Enhanced When In-Cloud Secondary Organic Aerosol is Included: Comparisons of Organic Carbon Predictions with Measurements [J].
Carlton, Annmarie G. ;
Turpin, Barbara J. ;
Altieri, Katye E. ;
Seitzinger, Sybil P. ;
Mathur, Rohit ;
Roselle, Shawn J. ;
Weber, Rodney J. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (23) :8798-8802
[3]   Modeling secondary organic aerosol formation through cloud processing of organic compounds [J].
Chen, J. ;
Griffin, R. J. ;
Grini, A. ;
Tulet, P. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2007, 7 (20) :5343-5355
[4]   Elemental analysis of chamber organic aerosol using an aerodyne high-resolution aerosol mass spectrometer [J].
Chhabra, P. S. ;
Flagan, R. C. ;
Seinfeld, J. H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (09) :4111-4131
[5]   Organic Aerosols in the Earth's Atmosphere [J].
De Gouw, Joost ;
Jimenez, Jose L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (20) :7614-7618
[6]   Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City [J].
Dzepina, K. ;
Volkamer, R. M. ;
Madronich, S. ;
Tulet, P. ;
Ulbrich, I. M. ;
Zhang, Q. ;
Cappa, C. D. ;
Ziemann, P. J. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (15) :5681-5709
[7]   Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles [J].
Ervens, B. ;
Volkamer, R. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (17) :8219-8244
[8]   Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols [J].
Fu, Tzung-May ;
Jacob, Daniel J. ;
Wittrock, Folkard ;
Burrows, John P. ;
Vrekoussis, Mihalis ;
Henze, Daven K. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D15)
[9]   Glyoxal uptake on ammonium sulphate seed aerosol: reaction products and reversibility of uptake under dark and irradiated conditions [J].
Galloway, M. M. ;
Chhabra, P. S. ;
Chan, A. W. H. ;
Surratt, J. D. ;
Flagan, R. C. ;
Seinfeld, J. H. ;
Keutsch, F. N. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (10) :3331-3345
[10]   Chemical evolution of secondary organic aerosol from OH-initiated heterogeneous oxidation [J].
George, I. J. ;
Abbatt, J. P. D. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (12) :5551-5563