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Published December 16, 2005 | Published + Supplemental Material
Journal Article Open

Chamber studies of secondary organic aerosol growth by reactive uptake of simple carbonyl compounds

Abstract

Recent experimental evidence indicates that heterogeneous chemical reactions play an important role in the gas-particle partitioning of organic compounds, contributing to the formation and growth of secondary organic aerosol in the atmosphere. Here we present laboratory chamber studies of the reactive uptake of simple carbonyl species (formaldehyde, octanal, trans,trans-2,4-hexadienal, glyoxal, methylglyoxal, 2,3-butanedione, 2,4-pentanedione, glutaraldehyde, and hydroxyacetone) onto inorganic aerosol. Gas-phase organic compounds and aqueous seed particles (ammonium sulfate or mixed ammonium sulfate/sulfuric acid) are introduced into the chamber, and particle growth and composition are monitored using a differential mobility analyzer and an Aerodyne Aerosol Mass Spectrometer. No growth is observed for most carbonyls studied, even at high concentrations (500 ppb to 5 ppm), in contrast with the results from previous studies. The single exception is glyoxal (CHOCHO), which partitions into the aqueous aerosol much more efficiently than its Henry's law constant would predict. No major enhancement in particle growth is observed for the acidic seed, suggesting that the large glyoxal uptake is not a result of particle acidity but rather of ionic strength of the seed. This increased partitioning into the particle phase still cannot explain the high levels of glyoxal measured in ambient aerosol, indicating that additional (possibly irreversible) pathways of glyoxal uptake may be important in the atmosphere.

Additional Information

© 2005 American Geophysical Union. Received 21 March 2005; revised 18 August 2005; accepted 19 September 2005; published 6 December 2005. This research was funded by U. S. Environmental Protection Agency Science to Achieve Results (STAR) Program grant RD-83107501-0, managed by EPA's Office of Research and Development (ORD), National Center for Environmental Research (NCER), and by U.S. Department of Energy Biological and Environmental Research Program DE-FG03-01ER63099. The authors are grateful to R. Bahreini for assistance with operation of the aerosol mass spectrometer; to A. Nenes for aid in calculating water content of the inorganic seed; to J. D. Crounse, C. M. Roehl, and P. O. Wennberg for the use of and aid with their FTIR spectrometer for the characterization of gas-phase glyoxal; and to B. Nozière and R. Volkamer for helpful discussions.

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Published - 232-Kroll-2005.pdf

Supplemental Material - jgrd12200-sup-0001-t01.txt

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