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Reactivity of polycyclic aromatic compounds (PAHs, NPAHs and OPAHs) adsorbed on natural aerosol particles exposed to atmospheric oxidants
Abstract Reactivity of polycyclic aromatic compounds (PACs) adsorbed on natural aerosol particles exposed to different atmospheric oxidants (O3, OH and NO2/O3 mixture) was studied. Decay of polycyclic aromatic hydrocarbons (PAHs) and formation/decay of oxygenated PAHs (OPAHs) and nitrated PAHs (NPAHs) were monitored. Overall, benzo[a]pyrene appeared to be the most reactive PAH (degradation of 50%). Only its nitrated derivative, 6-nitrobenzo[a]pyrene, was significantly formed explaining just 0.4% of reacted benzo[a]pyrene. No other nitrated or oxygenated benzo[a]pyrene derivatives were detected. Interestingly, B[e]P and In[1,2,3,c,d]P, which are usually considered as quite stable PAHs, also underwent decay in all experiments. In presence of O3, ketones were significantly formed but their amount was not totally explained by decay of parent PAH. These results suggest that PAH derivatives could be formed from the reaction of other compounds than their direct parent PAHs and raise the question to know if the oxidation of methyl-PAHs, identified in vehicle-exhausts, could constitute this missing source of OPAHs. NPAHs were significantly formed in presence of O3/NO2 and OH. Surprisingly, NPAH formation was clearly observed during O3 experiments. Nitrated species, already associated with aerosol particles (NO3 −, NO2 −) or formed by ozonation of particulate nitrogen organic matter, could react with PAHs to form NPAHs. Heterogeneous formation of 2-nitropyrene from pyrene oxidation was for the first time observed, questioning its use as an indicator of NPAH formation in gaseous phase. Equally, formation of 2-nitrofluoranthene by heterogeneous reaction of fluoranthene with O3/NO2 was clearly shown, while only its formation by homogeneous processes (gaseous phase) is reported in the literature. Finally, results obtained highlighted the dependence of heterogeneous PAH reactivity with the substrate nature and the importance to focus reactivity studies on natural particles, whatever the quality of the models previously studied.
Highlights ► We performed reactivity studies of PAC adsorbed on natural aerosol with OH, O3 or NO2. ► PAH degradations led to the formation of oxygenated and nitrated derivatives. ► Benzo[a]pyrene appeared as the most reactive PAH with all oxidants. ► Dependence of heterogeneous PAH reactivity with the substrate nature was highlighted. ► We showed the strong interest to work on natural aerosol particles from ambient air.
Reactivity of polycyclic aromatic compounds (PAHs, NPAHs and OPAHs) adsorbed on natural aerosol particles exposed to atmospheric oxidants
Abstract Reactivity of polycyclic aromatic compounds (PACs) adsorbed on natural aerosol particles exposed to different atmospheric oxidants (O3, OH and NO2/O3 mixture) was studied. Decay of polycyclic aromatic hydrocarbons (PAHs) and formation/decay of oxygenated PAHs (OPAHs) and nitrated PAHs (NPAHs) were monitored. Overall, benzo[a]pyrene appeared to be the most reactive PAH (degradation of 50%). Only its nitrated derivative, 6-nitrobenzo[a]pyrene, was significantly formed explaining just 0.4% of reacted benzo[a]pyrene. No other nitrated or oxygenated benzo[a]pyrene derivatives were detected. Interestingly, B[e]P and In[1,2,3,c,d]P, which are usually considered as quite stable PAHs, also underwent decay in all experiments. In presence of O3, ketones were significantly formed but their amount was not totally explained by decay of parent PAH. These results suggest that PAH derivatives could be formed from the reaction of other compounds than their direct parent PAHs and raise the question to know if the oxidation of methyl-PAHs, identified in vehicle-exhausts, could constitute this missing source of OPAHs. NPAHs were significantly formed in presence of O3/NO2 and OH. Surprisingly, NPAH formation was clearly observed during O3 experiments. Nitrated species, already associated with aerosol particles (NO3 −, NO2 −) or formed by ozonation of particulate nitrogen organic matter, could react with PAHs to form NPAHs. Heterogeneous formation of 2-nitropyrene from pyrene oxidation was for the first time observed, questioning its use as an indicator of NPAH formation in gaseous phase. Equally, formation of 2-nitrofluoranthene by heterogeneous reaction of fluoranthene with O3/NO2 was clearly shown, while only its formation by homogeneous processes (gaseous phase) is reported in the literature. Finally, results obtained highlighted the dependence of heterogeneous PAH reactivity with the substrate nature and the importance to focus reactivity studies on natural particles, whatever the quality of the models previously studied.
Highlights ► We performed reactivity studies of PAC adsorbed on natural aerosol with OH, O3 or NO2. ► PAH degradations led to the formation of oxygenated and nitrated derivatives. ► Benzo[a]pyrene appeared as the most reactive PAH with all oxidants. ► Dependence of heterogeneous PAH reactivity with the substrate nature was highlighted. ► We showed the strong interest to work on natural aerosol particles from ambient air.
Reactivity of polycyclic aromatic compounds (PAHs, NPAHs and OPAHs) adsorbed on natural aerosol particles exposed to atmospheric oxidants
Ringuet, Johany (author) / Albinet, Alexandre (author) / Leoz-Garziandia, Eva (author) / Budzinski, Hélène (author) / Villenave, Eric (author)
Atmospheric Environment ; 61 ; 15-22
2012-07-11
8 pages
Article (Journal)
Electronic Resource
English