Abstract
Air-liquid interfacial processing of volatile organic compound photooxidation has been suggested as an important source of secondary organic aerosols. However, owing to the lack of techniques for studying the air-liquid interface, the detailed interfacial mechanism remains speculative. To obviate this, we enabled in situ synchrotron-based vacuum ultraviolet single photon ionization mass spectrometry using the system for analysis at the liquid-vacuum interface microreactor to study glyoxal photooxidation at the air-liquid interface. Determination of reaction intermediates and new oxidation products, including polymers and oligomers, by mass spectral analysis and appearance energy measurements has been reported for the first time. Furthermore, an expanded reaction mechanism of photooxidation and free radical induced reactions as a source of aqueous secondary organic aerosol formation is proposed. Single photon ionization can provide new insights into interfacial chemistry.
| Original language | English |
|---|---|
| Pages (from-to) | 324-329 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 12 |
| Issue number | 1 |
| DOIs | |
| State | Published - Jan 14 2021 |
Funding
XS is grateful for the support from Pacific Northwest National Laboratory (PNNL) Alternate Sponsored Fellowship (ASF). X-Y Y and JY were grateful for the support from the PNNL Earth and Biological Science Directorate (EBSD) mission seed Laboratory Directed Research and Development (LDRD) support to perform beamline experiments. X-Y Y thanks Office of Science, Office of Basic Energy Sciences, of the U.S. DOE through the Direct Air Capture Program for partial support in writing this manuscript. 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. BX, OK, and MA are supported by 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. PNNL is operated for the U.S. DOE by Battelle Memorial Institute under Contract No. DE-AC05-76RL01830. The authors thank Miss Rachel Komorek, Dr. Fei Zhang, Dr. Jiachao Yu, and Dr. Tyler Troy for device fabrication, sample preparation, and experimental assistance.