Kinetics, Products, and Brown Carbon Formation by Aqueous-Phase Reactions of Glycolaldehyde with Atmospheric Amines and Ammonium Sulfate

Rodriguez, Alyssa A.; Rafla, Michael A.; Welsh, Hannah G.; Pennington, Elyse A.; Casar, Jason R.; Hawkins, Lelia N.; Jimenez, Natalie G.; de Loera, Alexia; Stewart, Devoun R.; Rojas, Antonio; Tran, Matthew-Khoa; Lin, Peng; Laskin, Alexander; Formenti, Paola; Cazaunau, Mathieu; Pangui, Edouard; Doussin, Jean-François; De Haan, David O.

doi:10.1021/acs.jpca.2c02606

Kinetics, Products, and Brown Carbon Formation by Aqueous-Phase Reactions of Glycolaldehyde with Atmospheric Amines and Ammonium Sulfate

Journal Article · Thu Aug 04 00:00:00 EDT 2022 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.2c02606· OSTI ID:2469845

Rodriguez, Alyssa A. ^[1]; Rafla, Michael A. ^[1]; Welsh, Hannah G. ^[2]; Pennington, Elyse A. ^[2]; ^[2]; ^[2]; Jimenez, Natalie G. ^[1]; de Loera, Alexia ^[1]; Stewart, Devoun R. ^[1]; Rojas, Antonio ^[1]; Tran, Matthew-Khoa ^[1]; Lin, Peng ^[3]; ^[3]; Formenti, Paola ^[4]; Cazaunau, Mathieu ^[4]; Pangui, Edouard ^[4]; Doussin, Jean-François ^[4]; ^[1]

Univ. of San Diego, CA (United States)
Harvey Mudd College, Claremont, CA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); Purdue Univ., West Lafayette, IN (United States)
Université Paris-Est Créteil (UPEC) (France); Univ. of Paris (France); Centre National de la Recherche Scientifique (CNRS) (France)

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.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2469845

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 32 Vol. 126; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Kinetics, Products, and Brown Carbon Formation by Aqueous-Phase Reactions of Glycolaldehyde with Atmospheric Amines and Ammonium Sulfate

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