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Evolution of aqSOA from the Air–Liquid Interfacial Photochemistry of Glyoxal and Hydroxyl Radicals

Journal Article · · Environmental Science and Technology
 [1];  [2];  [2];  [3];  [2];  [2]
  1. Fudan Univ., Shanghai (China); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Fudan Univ., Shanghai (China)
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The effect of photochemical reaction time on glyoxal and hydrogen peroxide at the aqueous surface is investigated using in situ time-of-flights Secondary ion mass spectrometry (ToF-SIMS) enabled by a system for analysis at the liquid vacuum interface (SALVI) microreactor. Carboxylic acids (i.e., glyoxylic acid, oxalic acid, malonic acid, tartaric acid) are observed in the initial reactions (i.e., < 3 h.), more oligomers, cluster ions, and water clusters formed in the long ultraviolet (UV) aging period (i.e., = 3 h). Our results provide the direct evidence that water clusters could promote proton transfer and facilitate the formation of oligomers and cluster ions in the aqeous environment as photochemical aging continues. Furthermore, new chemical reaction pathways are proposed to expand existing understanding. The temporal evolution shows that oxidation products such as carboxylic acids reach a maximum in 1 h, whereas oligomer yields peak in 3 to 4 h. Glyoxal not only undergoes oxidation to form carboxylic acids (mainly occurred in the aging time less than 3 h), but also takes part in radical reactions, hemiacetal, oligomerization, polymerization, esterification, and anhydride reactions to form higher molecular weight species. Our in situ findings verify that the air-liquid interfacial reactions are important pathways for aqueous secondary organic aerosol (aqSOA) formation.
Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1572949
Report Number(s):
PNNL-SA--135488
Journal Information:
Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 17 Vol. 53; ISSN 0013-936X
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

Figures / Tables (6)

Figure 1(p. 23)figure Figure 1
Figure 2(p. 24)figure Figure 2
Figure 3(p. 25)figure Figure 3
Figure 4(p. 26)figure Figure 4
Figure 5(p. 27)figure Figure 5
Table 1(p. 28)table Table 1

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
aqueous SOA
cluster ions
glyoxal
in situ liquid SIMS
surface mixing state