Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 53, Issue 17, Pages 10236-10245Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.9b03642
Keywords
-
Categories
Funding
- Pacific Northwest National Laboratory (PNNL), Materials Synthesis and Simulation across Scales (MS3)
- Initiative Laboratory Directed Research and Development (LDRD)
- National Natural Science Foundation of China [21527814]
- Ministry of Science and Technology of China [2016YFC0202700, 2016YFE0112200, 2014BAC22B01]
- Marie Sklodowska-Curie Actions [690958-MARSU-RISE-2015]
- office of Biological and Environmental Research (OBER)
- China Scholarship Council (CSC)
- Earth and Biological Sciences Directorate (EBSD)
- Mission Seed LDRD
- PNNL Alternate Sponsored Fellowship (ASF)
Ask authors/readers for more resources
The effect of photochemical reaction time on glyoxal and hydrogen peroxide at the air-liquid (a-l) interface is investigated using in situ time-of-flight secondary ion mass spectrometry (ToF-SIMS) enabled by a system for analysis at the liquid vacuum interface (SALVO microreactor. Carboxylic acids are formed mainly by reaction with hydroxyl radicals in the initial reactions. Oligomers, cluster ions, and water clusters formed due to longer photochemistry. Our results provide direct molecular evidence that water clusters are associated with proton transfer and the formation of oligomers and cluster ions at the a-l interface. The oligomer formation is facilitated by water cluster and cluster ion formation over time. Formation of higher m/z oligomers and cluster ions indicates the possibility of highly oxygenated organic components formation at the a-l interface. Furthermore, new chemical reaction pathways, such as surface organic cluster, hydration shell, and water cluster formation, are proposed based on SIMS spectral observations, and the existing understanding of glyoxal photochemistry is expanded. Our in situ findings verify that the a-l interfacial reactions are important pathways for aqueous secondary organic aerosol (aqSOA) formation.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available