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Reactive Uptake and Photo-Fenton Oxidation of Glycolaldehyde in Aerosol Liquid Water

Nguyen, T. B. and Coggon, M. M. and Flagan, R. C. and Seinfeld, J. H. (2013) Reactive Uptake and Photo-Fenton Oxidation of Glycolaldehyde in Aerosol Liquid Water. Environmental Science and Technology, 47 (9). pp. 4307-4316. ISSN 0013-936X. https://resolver.caltech.edu/CaltechAUTHORS:20130703-095608075

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Abstract

The reactive uptake and aqueous oxidation of glycolaldehyde were examined in a photochemical flow reactor using hydrated ammonium sulfate (AS) seed aerosols at RH = 80%. The glycolaldehyde that partitioned into the aerosol liquid water was oxidized via two mechanisms that may produce aqueous OH: hydrogen peroxide photolysis (H_(2)O_(2) + hν) and the photo-Fenton reaction (Fe_(II) + H_(2)O_(2) + hν). The uptake of 80 (±10) ppb glycolaldehyde produced 2–4 wt % organic aerosol mass in the dark (k_(H)* = (2.09–4.17) × 10^6 M atm^(–1)), and the presence of an OH source increased the aqueous uptake by a factor of 4. Although the uptake was similar in both OH-aging mechanisms, photo-Fenton significantly increased the degree of oxidation (O/C = 0.9) of the aerosols compared to H_(2)O_(2) photolysis (O/C = 0.5). Aerosol organics oxidized by photo-Fenton and H_(2)O_(2) photolysis resemble ambient “aged” and “fresh” OA, respectively, after the equivalent of 2 h atmospheric aging. No uptake or changes in particle composition occurred on dry seed aerosol. This work illustrates that photo-Fenton chemistry efficiently forms highly oxidized organic mass in aerosol liquid water, providing a possible mechanism to bridge the gap between bulk-phase experiments and ambient particles.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/es400538jDOIArticle
https://doi.org/10.1021/es403622yDOICorrection
https://pubs.acs.org/doi/suppl/10.1021/es400538jPublisherSupporting Information
ORCID:
AuthorORCID
Coggon, M. M.0000-0002-5763-1925
Flagan, R. C.0000-0001-5690-770X
Seinfeld, J. H.0000-0003-1344-4068
Additional Information:© 2013 American Chemical Society. Received: February 2, 2013; Revised: April 2, 2013; Accepted: April 4, 2013; Published: April 4, 2013. This research was supported by the National Science Foundation grant AGS-1057183. T. B. Nguyen acknowledges funding from the Coco and Foster Stanback Postdoctoral Fellowship in Global Environmental Science. We are grateful to Prof. S. A. Nizkorodov (UC Irvine) for his contribution of a portion of the equipment used in this work. We thank Prof. P. O. Wennberg and Prof. M. R. Hoffman for helpful discussions.
Errata:The Henry’s law constant (k_H) of glycolaldehyde, adapted from Betterton and Hoffmann (1988), should have been written as 4.14 × 10^4 M atm^(-1) instead of 4.14 × 10^5 M atm^(-1).
Funders:
Funding AgencyGrant Number
NSFAGS-1057183
Coco and Foster Stanback Postdoctoral Fellowship in Global Environmental ScienceUNSPECIFIED
Issue or Number:9
Record Number:CaltechAUTHORS:20130703-095608075
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20130703-095608075
Official Citation:Reactive Uptake and Photo-Fenton Oxidation of Glycolaldehyde in Aerosol Liquid Water T. B. Nguyen, M. M. Coggon, R. C. Flagan, and J. H. Seinfeld Environmental Science & Technology 2013 47 (9), 4307-4316
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:39199
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:08 Jul 2013 22:49
Last Modified:03 Oct 2019 05:04

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