Document Type

Article

Publication Date

Summer 8-4-2022

Journal Title

The Journal of Physical Chemistry A

First Page

A

Last Page

K

DOI

https://doi.org/10.1021/acs.jpca.2c02606

Version

Publisher PDF: the final published version of the article, with professional formatting and typesetting

Disciplines

Chemistry | Physical Chemistry

Abstract

Glycolaldehyde (GAld) is a C2 water-soluble aldehyde produced during the atmospheric oxidation of isoprene and many other species and is commonly found in cloudwater. Previous work has established that glycolaldehyde evaporates more readily from drying aerosol droplets containing ammonium sulfate (AS) than does glyoxal, methylglyoxal, or hydroxyacetone, which implies that it does not oligomerize as quickly as these other species. Here, we report NMR measurements of glycolaldehyde’s aqueous-phase reactions with AS, methylamine, and glycine. Reaction rate constants are smaller than those of respective glyoxal and methylglyoxal reactions in the pH range of 3–6. In follow-up cloud chamber experiments, deliquesced glycine and AS seed particles were found to take up glycolaldehyde and methylamine and form brown carbon. At very high relative humidity, these changes were more than 2 orders of magnitude faster than predicted by our bulk liquid NMR kinetics measurements, suggesting that reactions involving surface-active species at crowded air–water interfaces may play an important role. The high-resolution liquid chromatography–electrospray ionization–mass spectrometric analysis of filter extracts of unprocessed AS + GAld seed particles identified sugar-like C6 and C12 GAld oligomers, including proposed product 3-deoxyglucosone, with and without modification by reactions with ammonia to diimine and imidazole forms. Chamber exposure to methylamine gas, cloud processing, and simulated sunlight increased the incorporation of both ammonia and methylamine into oligomers. Many C4–C16 imidazole derivatives were detected in an extract of chamber-exposed aerosol along with a predominance of N-derivatized C6 and C12 glycolaldehyde oligomers, suggesting that GAld is capable of forming brown carbon SOA.

Notes

Original publication information: 'Kinetics, Products, and Brown Carbon Formation by Aqueous-Phase Reactions of Glycolaldehyde with Atmospheric Amines and Ammonium Sulfate', Alyssa A. Rodriguez, Michael A. Rafla, Hannah G. Welsh, Elyse A. Pennington, Jason R. Casar, Lelia N. Hawkins, Natalie G. Jimenez, Alexia de Loera, Devoun R. Stewart, Antonio Rojas, Matthew-Khoa Tran, Peng Lin, Alexander Laskin, Paola Formenti, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and David O. De Haan, The Journal of Physical Chemistry A.

DOI: 10.1021/acs.jpca.2c02606

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