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Brown Carbon Production in Ammonium- or Amine-Containing Aerosol Particles by Reactive Uptake of Methylglyoxal and Photolytic Cloud Cycling

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Department of Chemistry and Biochemistry, University of San Diego, 5998 Alcala Park, San Diego, California 92110, United States
Department of Chemistry, Harvey Mudd College, 301 Platt Blvd, Claremont, California 91711, United States
§ Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, 70211 Kuopio, Finland
Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), UMR7583, CNRS, Université Paris-Est-Créteil (UPEC) et Université Paris Diderot (UPD), Institut Pierre Simon Laplace (IPSL), 94010 Créteil, France
*Phone: (619) 260-6882. Fax: (619) 260-2211. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2017, 51, 13, 7458–7466
Publication Date (Web):May 31, 2017
https://doi.org/10.1021/acs.est.7b00159
Copyright © 2017 American Chemical Society

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    Abstract

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    The effects of methylglyoxal uptake on the physical and optical properties of aerosol containing amines or ammonium sulfate were determined before and after cloud processing in a temperature- and RH-controlled chamber. The formation of brown carbon was observed upon methylglyoxal addition, detected as an increase in water-soluble organic carbon mass absorption coefficients below 370 nm and as a drop in single-scattering albedo at 450 nm. The imaginary refractive index component k450 reached a maximum value of 0.03 ± 0.009 with aqueous glycine aerosol particles. Browning of solid particles occurred at rates limited by chamber mixing (<1 min), and in liquid particles occurred more gradually, but in all cases occurred much more rapidly than in bulk aqueous studies. Further browning in AS and methylammonium sulfate seeds was triggered by cloud events with chamber lights on, suggesting photosensitized brown carbon formation. Despite these changes in optical aerosol characteristics, increases in dried aerosol mass were rarely observed (<1 μg/m3 in all cases), consistent with previous experiments on methylglyoxal. Under dry, particle-free conditions, methylglyoxal reacted (presumably on chamber walls) with methylamine with a rate constant k = (9 ± 2) × 10–17 cm3 molecule–1 s–1 at 294 K and activation energy Ea = 64 ± 37 kJ/mol.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b00159.

    • Pressure, temperature, and PTR-MS data for other m/z ratios for each chamber experiment; a sample CAPS calibration; SMPS pre- and postcloud aerosol size distributions; bounce fraction data for methylamine sulfate and three other particle types; graphs of time-dependent imaginary components of the index of refraction; data from an AS + cloud control experiment; discussion of albedo baselines and excursions measured between baseline events; aerosol density and phase; aerosol and chamber cloud lifetimes; and aerosol bounce measurements (PDF)

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