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Aqueous-Phase Photoreactions of Mixed Aromatic Carbonyl Photosensitizers Yield More Oxygenated, Oxidized, and less Light-Absorbing Secondary Organic Aerosol (SOA) than Single Systems
Mabato, Beatrix Rosette Go1; Li, Yong Jie2; Huang, Dan Dan3; Chan, Chak K.1,4
2024-04-23
Source PublicationENVIRONMENTAL SCIENCE & TECHNOLOGY
ABS Journal Level3
ISSN0013-936X
Volume58Issue:18Pages:7924-7936
Abstract

Aromatic carbonyls have been mainly probed as photosensitizers for aqueous secondary organic aerosol (aqSOA) and light-absorbing organic aerosol (i.e., brown carbon or BrC) formation, but due to their organic nature, they can also undergo oxidation to form aqSOA and BrC. However, photochemical transformations of aromatic carbonyl photosensitizers, particularly in multicomponent systems, are understudied. This study explored aqSOA formation from the irradiation of aromatic carbonyl photosensitizers in mixed and single systems under cloud/fog conditions. Mixed systems consisting of phenolic carbonyls only (VL + ActSyr + SyrAld: vanillin [VL] + acetosyringone [ActSyr] + syringaldehyde [SyrAld]) and another composed of both nonphenolic and phenolic carbonyls (DMB + ActSyr + SyrAld: 3,4-dimethoxybenzaldehyde [DMB], a nonphenolic carbonyl, + ActSyr + SyrAld) were compared to single systems of VL (VL*) and DMB (DMB*), respectively. In mixed systems, the shorter lifetimes of VL and DMB indicate their diminished capacity to trigger the oxidation of other organic compounds (e.g., guaiacol [GUA], a noncarbonyl phenol). In contrast to the slow decay and minimal photoenhancement for DMB*, the rapid photodegradation and significant photoenhancement for VL* indicate efficient direct photosensitized oxidation (i.e., self-photosensitization). Relative to single systems, the increased oxidant availability promoted functionalization in VL + ActSyr + SyrAld and accelerated the conversion of early generation aqSOA in DMB + ActSyr + SyrAld. Moreover, the increased availability of oxidizable substrates countered by stronger oxidative capacity limited the contribution of mixed systems to aqSOA light absorption. This suggests a weaker radiative effect of BrC from mixed photosensitizer systems than BrC from single photosensitizer systems. Furthermore, more oxygenated and oxidized aqSOA was observed with increasing complexity of the reaction systems (e.g., VL* < VL + ActSyr + SyrAld < VL + ActSyr + SyrAld + GUA). This work offers new insights into aqSOA formation by emphasizing the dual role of organic photosensitizers as oxidant sources and oxidizable substrates.

KeywordAqueous Secondary Organic Aerosol Aromatic Carbonyl Photosensitizers Light Absorption, Brown Carbon (Brc) Mixed Photosensitizer System Photosensitization
DOI10.1021/acs.est.3c10199
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaEngineering ; Environmental Sciences & Ecology
WOS SubjectEngineering, Environmental ; Environmental Sciences
WOS IDWOS:001227688100001
PublisherAMER CHEMICAL SOC, 1155 16TH ST, NW, WASHINGTON, DC 20036
Scopus ID2-s2.0-85191877965
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Citation statistics
Document TypeJournal article
CollectionFaculty of Science and Technology
DEPARTMENT OF CIVIL AND ENVIRONMENTAL ENGINEERING
Corresponding AuthorChan, Chak K.
Affiliation1.School of Energy and Environment, City University of Hong Kong, Kowloon, Tat Chee Avenue, Hong Kong SAR, 999077, Hong Kong
2.Department of Civil and Environmental Engineering, and Centre for Regional Ocean, Faculty of Science and Technology, University of Macau, Macau, 999078, Macao
3.Shanghai Academy of Environmental Sciences, Shanghai, 200233, China
4.Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal, Jeddah, 23955-6900, Saudi Arabia
Recommended Citation
GB/T 7714
Mabato, Beatrix Rosette Go,Li, Yong Jie,Huang, Dan Dan,et al. Aqueous-Phase Photoreactions of Mixed Aromatic Carbonyl Photosensitizers Yield More Oxygenated, Oxidized, and less Light-Absorbing Secondary Organic Aerosol (SOA) than Single Systems[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2024, 58(18), 7924-7936.
APA Mabato, Beatrix Rosette Go., Li, Yong Jie., Huang, Dan Dan., & Chan, Chak K. (2024). Aqueous-Phase Photoreactions of Mixed Aromatic Carbonyl Photosensitizers Yield More Oxygenated, Oxidized, and less Light-Absorbing Secondary Organic Aerosol (SOA) than Single Systems. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 58(18), 7924-7936.
MLA Mabato, Beatrix Rosette Go,et al."Aqueous-Phase Photoreactions of Mixed Aromatic Carbonyl Photosensitizers Yield More Oxygenated, Oxidized, and less Light-Absorbing Secondary Organic Aerosol (SOA) than Single Systems".ENVIRONMENTAL SCIENCE & TECHNOLOGY 58.18(2024):7924-7936.
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