Studying interfacial dark reactions of Glyoxal and hydrogen peroxide using vacuum ultraviolet single photon ionization mass spectrometry

Xiao Sui; Bo Xu; Jiachao Yu; Oleg Kostko; Musahid Ahmed; Xiao Ying Yu

doi:10.3390/atmos12030338

Studying interfacial dark reactions of Glyoxal and hydrogen peroxide using vacuum ultraviolet single photon ionization mass spectrometry

Xiao Sui, Bo Xu, Jiachao Yu, Oleg Kostko, Musahid Ahmed, Xiao Ying Yu

Advanced Nuclear Materials

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

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.

Original language	English
Article number	338
Journal	Atmosphere
Volume	12
Issue number	3
DOIs	https://doi.org/10.3390/atmos12030338
State	Published - Mar 2021

Funding

Acknowledgments: X.S. is grateful for the support from the PNNL Alternate Sponsored Fellowship (ASF). The authors thank Rachel Komorek, Jenn Yao, Fei Zhang, and Tyler Troy for their assistance in device fabrication, sample preparation, and data analysis. Funding: The programmatic support of the experimental work for X.Y.Y. and J.Y. was from Pacific Northwest National Laboratory (PNNL), the Earth and Biological Science Directorate (EBSD), and mission seed Laboratory Directed Research and Development (LDRD) support to perform the beamline experiment. The manuscript preparation for X.Y.Y. was supported partially by the Physical and Computational Science Directorate (PCSD) LDRD. PNNL is operated for the U.S. DOE by Battelle Memorial Institute under Contract No. DE-AC05-76RL01830. This research used resources of the Advanced Light Source, a Department of Energy (DOE) Office of Science User Facility under contract no. DE-AC02-05CH11231. Programmatic support for B.X., O.K., and M.A. was from the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. DOE under Contract No. DE-AC02-05CH11231, through the Gas Phase Chemical Physics Program and Condensed Phase, Interfaces, and Molecular Sciences Program.

Keywords

Air-liquid interfacial reactions
Aqueous secondary organic aerosol
Dark aging
Glyoxal
Hydrogen peroxide
SALVI
VUV SPI-MS

Access to Document

10.3390/atmos12030338

Cite this

@article{628def28993843d4b912be294216f38d,

title = "Studying interfacial dark reactions of Glyoxal and hydrogen peroxide using vacuum ultraviolet single photon ionization mass spectrometry",

abstract = "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.",

keywords = "Air-liquid interfacial reactions, Aqueous secondary organic aerosol, Dark aging, Glyoxal, Hydrogen peroxide, SALVI, VUV SPI-MS",

author = "Xiao Sui and Bo Xu and Jiachao Yu and Oleg Kostko and Musahid Ahmed and Yu, \{Xiao Ying\}",

note = "Publisher Copyright: {\textcopyright} 2021 by the authors. Licensee MDPI, Basel, Switzerland.",

year = "2021",

month = mar,

doi = "10.3390/atmos12030338",

language = "English",

volume = "12",

journal = "Atmosphere",

issn = "2073-4433",

publisher = "MDPI",

number = "3",

}

TY - JOUR

T1 - Studying interfacial dark reactions of Glyoxal and hydrogen peroxide using vacuum ultraviolet single photon ionization mass spectrometry

AU - Sui, Xiao

AU - Xu, Bo

AU - Yu, Jiachao

AU - Kostko, Oleg

AU - Ahmed, Musahid

AU - Yu, Xiao Ying

PY - 2021/3

Y1 - 2021/3

N2 - 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.

AB - 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.

KW - Air-liquid interfacial reactions

KW - Aqueous secondary organic aerosol

KW - Dark aging

KW - Glyoxal

KW - Hydrogen peroxide

KW - SALVI

KW - VUV SPI-MS

UR - https://www.scopus.com/pages/publications/85102753965

U2 - 10.3390/atmos12030338

DO - 10.3390/atmos12030338

M3 - Article

AN - SCOPUS:85102753965

SN - 2073-4433

VL - 12

JO - Atmosphere

JF - Atmosphere

IS - 3

M1 - 338

ER -

Studying interfacial dark reactions of Glyoxal and hydrogen peroxide using vacuum ultraviolet single photon ionization mass spectrometry

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this