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Photoenhanced Uptake of NO 2 by Pyrene Solid Films

2008; American Chemical Society; Volume: 112; Issue: 39 Linguagem: Inglês

10.1021/jp802324g

1520-5215

Marcello Brigante, David Cazoir, Barbara D’Anna, C. George, D. J. Donaldson,

Air Quality and Health Impacts

We report uptake kinetics measurements of the heterogeneous reaction of gas phase NO2 with solid films of pyrene. By using a coated flow tube equipped with several near-ultraviolet (UV) emitting lamps (range 300-420 nm), we examined the effect of actinic radiation on the heterogeneous loss kinetics of nitrogen dioxide. With atmospherically relevant concentrations of NO2, (20-119 ppbv), the uptake ranged from below 10(-7) in the dark to 3.5 x 10(-6) under near-UV irradiation. Under illuminated conditions, the uptake coefficient decreased markedly with increasing gas-phase concentration, suggestive of a Langmuir-Hinshelwood-type surface reaction mechanism. The NO2 reactivity was not a function of deposited Pyrene mass or of the relative humidity (in the range 10-89%) and depended linearly on the intensity of illumination. Gas-phase product analysis indicated that approximately 50% of the NO2 loss could be accounted for by HONO and NO release. These experimental results are discussed along with a possible nitration mechanism.