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Studying Interfacial Dark Reactions of Glyoxal and Hydrogen Peroxide Using Vacuum Ultraviolet Single Photon Ionization Mass Spectrometry

Journal Article · · Atmosphere (Basel)
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Aqueous secondary organic aerosol (aqSOA) formation from volatile and semivolatile organic compounds at the air–liquid interface is considered as an important source of fine particles in the atmosphere. However, due to the lack of in situ detecting techniques, the detailed interfacial reaction mechanism and dynamics still remain uncertain. In this study, synchrotron-based vacuum ultraviolet single-photon ionization mass spectrometry (VUV SPI-MS) was coupled with the System for Analysis at the Liquid Vacuum Interface (SALVI) to investigate glyoxal dark oxidation products at the aqueous surface. Mass spectral analysis and determination of appearance energies (AEs) suggest that the main products of glyoxal dark interfacial aging are carboxylic acid related oligomers. Furthermore, the VUV SPI-MS results were compared and validated against those of in situ liquid time-of-flight secondary ion mass spectrometry (ToF-SIMS). The reaction mechanisms of the dark glyoxal interfacial oxidation, obtained using two different approaches, indicate that differences in ionization and instrument operation principles could contribute to their abilities to detect different oligomers. Therefore, the mechanistic differences revealed between the VUV SPI-MS and ToF-SIMS indicate that more in situ and real-time techniques are needed to investigate the contribution of the air–liquid interfacial reactions leading to aqSOA formation.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC02-05CH11231; AC05-76RL01830
OSTI ID:
1769516
Alternate ID(s):
OSTI ID: 1813359
OSTI ID: 1785533
Report Number(s):
PNNL-SA--160248; PII: atmos12030338
Journal Information:
Atmosphere (Basel), Journal Name: Atmosphere (Basel) Journal Issue: 3 Vol. 12; ISSN 2073-4433; ISSN ATMOCZ
Publisher:
MDPI AGCopyright Statement
Country of Publication:
Switzerland
Language:
English

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Evolution of aqSOA from the Air–Liquid Interfacial Photochemistry of Glyoxal and Hydroxyl Radicals
Journal Article · Mon Jul 29 20:00:00 EDT 2019 · Environmental Science and Technology · OSTI ID:1572949

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
SALVI
air-liquid interfacial reactions
aqueous secondary organic aerosol
dark aging
glyoxal
hydrogen peroxide