Abstract
This work deals with the kinetic study of the reactions of ozone with pyrene, 1-hydroxypyrene and 1-nitropyrene, adsorbed on model particles. Experiments were performed at room temperature and atmospheric pressure, using a quasi-static flow reactor in the absence of light. Compounds were extracted from particles using pressurized fluid extraction (PFE) and concentration measurements were performed using gas chromatography/mass spectrometry (GC/MS). The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate polycyclic compound concentrations versus reaction time. Experiments were performed at three different O 3 concentrations from which second order rate constants were calculated. The following rate constant values were obtained at 293 K: k(O 3 + Pyrene) = (3.2 ± 0.7) × 10 −16 cm 3 molecule −1 s −1; k(O 3 + 1OHP) = (7.7 ± 1.4) ×10 −16 cm 3 molecule −1 s −1; and k(O 3 + 1NP) = (2.2 ± 0.5) × 10 −17 cm 3 molecule −1 s −1, for pyrene, 1-hydroxypyrene and 1-nitropyrene adsorbed on silica particles. The variation in the rate constants demonstrates the strong influence of the substituent (OH or NO 2) on the heterogeneous reactivity of pyrene. The pyrene particulate concentration was also varied in order to check how this parameter may influence the experiments. Finally, oxidation products were investigated for all reactions and some were detected and identified for the first time for ozone heterogeneous reaction with pyrene adsorbed on particles.
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