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Secondary organic aerosol formation from the photo-oxidation of benzene
Abstract The production of condensate compounds from the degradation of benzene by OH radical chemistry was studied. Secondary organic aerosol (SOA) formation was investigated in the EUPHORE (European Photoreactor) simulation chambers. Experiments were performed under different OH-production conditions – addition of H2O2, NO or HONO –, in a high-volume reactor, with natural light and in the absence of seed aerosols. The consumption of precursor/reagents, the formation of gas-phase and particulate-phase products and the temporal evolution of aerosol were monitored. Several aerosol physical properties – mass concentration, overall aerosol yield, particle size distribution and density – were determined and found to be clearly dependent on OH radical production and NOx concentrations. Furthermore, the use of one and/or two products gas-particle partitioning absorption models allowed us to determine the aerosol yield curves. The SOA yield ranged from 1.6 to 9.7 %, with higher SOA formation under low-NOx conditions. Chemical characterization of the SOA was carried out, determining multi-oxygenated condensed organic compounds by a method based on the gas chromatography-mass spectrometry technique. Several ring-retaining and ring-cleavage products were identified and quantified. The compounds with the highest percentage contribution to the total aerosol mass were 4-nitrobenzene-1,2-diol, butenedioic acid, succinic acid and trans-trans-muconic. In addition, a multigenerational study was performed comparing with the photo-oxidations of phenol and catechol. The results showed that although the mass concentration of SOA produced was different, the physical and chemical properties were quite similar. Finally, we suggest a general mechanism to describe how changes in benzene degradation pathways – rate of OH generation and concentration of NOx – could justify the variation in SOA production and properties.
Graphical abstract Display Omitted Highlights ► SOA yields from the photo-oxidation of benzene, phenol and catechol were 1.6–53%. ► Mass concentration, size distribution, density and composition were determined. ► Aerosol properties were found clearly dependent on OH production and NOx levels. ► Yield models informed about the source and nature of SOA intermediates. ► Multi-oxygenated products (ring-cleavage/ring-retaining) are relevant SOA components.
Secondary organic aerosol formation from the photo-oxidation of benzene
Abstract The production of condensate compounds from the degradation of benzene by OH radical chemistry was studied. Secondary organic aerosol (SOA) formation was investigated in the EUPHORE (European Photoreactor) simulation chambers. Experiments were performed under different OH-production conditions – addition of H2O2, NO or HONO –, in a high-volume reactor, with natural light and in the absence of seed aerosols. The consumption of precursor/reagents, the formation of gas-phase and particulate-phase products and the temporal evolution of aerosol were monitored. Several aerosol physical properties – mass concentration, overall aerosol yield, particle size distribution and density – were determined and found to be clearly dependent on OH radical production and NOx concentrations. Furthermore, the use of one and/or two products gas-particle partitioning absorption models allowed us to determine the aerosol yield curves. The SOA yield ranged from 1.6 to 9.7 %, with higher SOA formation under low-NOx conditions. Chemical characterization of the SOA was carried out, determining multi-oxygenated condensed organic compounds by a method based on the gas chromatography-mass spectrometry technique. Several ring-retaining and ring-cleavage products were identified and quantified. The compounds with the highest percentage contribution to the total aerosol mass were 4-nitrobenzene-1,2-diol, butenedioic acid, succinic acid and trans-trans-muconic. In addition, a multigenerational study was performed comparing with the photo-oxidations of phenol and catechol. The results showed that although the mass concentration of SOA produced was different, the physical and chemical properties were quite similar. Finally, we suggest a general mechanism to describe how changes in benzene degradation pathways – rate of OH generation and concentration of NOx – could justify the variation in SOA production and properties.
Graphical abstract Display Omitted Highlights ► SOA yields from the photo-oxidation of benzene, phenol and catechol were 1.6–53%. ► Mass concentration, size distribution, density and composition were determined. ► Aerosol properties were found clearly dependent on OH production and NOx levels. ► Yield models informed about the source and nature of SOA intermediates. ► Multi-oxygenated products (ring-cleavage/ring-retaining) are relevant SOA components.
Secondary organic aerosol formation from the photo-oxidation of benzene
Borrás, Esther (author) / Tortajada-Genaro, Luis Antonio (author)
Atmospheric Environment ; 47 ; 154-163
2011-11-07
10 pages
Article (Journal)
Electronic Resource
English