Synergistic generation mechanisms of SOA and ozone from the photochemical oxidation of 1,3,5-trimethylbenzene: Influence of precursors ratio, temperature and radiation intensity

Atmospheric Research(2023)

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摘要
Aromatic hydrocarbons (AHs) are important anthropogenic precursors for both secondary organic aerosol (SOA) and ozone (O3) in urban areas. Knowledge about the synergistic processes and influence mechanisms of SOA and O3 during the photochemical oxidation of AHs is still relatively limited. In this study, the synergistic formation processes of SOA and O3 through the photochemical reactions of a representative AHs (1,3,5-trimethylbenzene, 135TMB) under different initial volatile organic compound/nitrogen oxides ([VOC]/[NOX]) ratios, temperatures and radiation intensities were investigated. The results showed that temperature and radiation significantly affected the reaction products and yields: the O3 production rates under high temperatures and radiation were greater than those under low temperatures and radiation, whereas the mass concentrations and yields of SOA under low temperatures and radiation were much higher than those under high temperatures and radiation. It was also found that the SOA yield increased with increasing NOX concentration within a specific initial [135TMB]/[NOX] ratio, but it decreased with increasing NOX concentration beyond a specific initial [135TMB]/[NOX] ratio. In addition, the concentrations of SOA and O3 in all the experiments increased simultaneously regardless of low temperatures or high temperatures. From these phenomena, it can be inferred that appropriate strategies for O3 precursor abatement can simultaneously reduce the concentration of SOA, which means that the coordinated control of fine particles and O3 could be achieved by taking coordinated emission reduction measures for VOCs and NOX precursors. The analysis of the organic components revealed that intramolecular hydrogen transfer occurred in some reactions in 135TMB photooxidation, and low-volatility and high-oxidative state organics were formed. The master chemical mechanism (MCM) results showed that the existing MCM mechanism does not yet fully meet the need to simulate the atmospheric photochemical reaction processes of 135TMB in the real atmosphere in China, and a localized MCM mechanism needs to be developed in the future.
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关键词
1,3,5-Trimethylbenzene (135TMB),Secondary organic aerosol (SOA),Ozone,Coordinated formation mechanisms,Outdoor smog chamber,MCM simulation
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