[1] Airborne formaldehyde (CH 2 O) measurements were made by tunable diode laser absorption spectroscopy (TDLAS) at high time resolution (1 and 10 s) and precision (±400 and ±120 parts per trillion by volume (pptv) (2s), respectively) during the Texas Air Quality Study (TexAQS) 2000. Measurement accuracy was corroborated by in-flight calibrations and zeros and by overflight comparison with a ground-based differential optical absorption spectroscopy (DOAS) system. Throughout the campaign, the highest levels of CH 2 O precursors and volatile organic compound (VOC) reactivity were measured in petrochemical plumes. Correspondingly, CH 2 O and ozone production was greatly enhanced in petrochemical plumes compared with plumes dominated by power plant and mobile source emissions. The photochemistry of several isolated petrochemical facility plumes was accurately modeled using three nonmethane hydrocarbons (NMHCs) (ethene (C 2 H 4 ), propene (C 3 H 6 ) (both anthropogenic), and isoprene (C 5 H 8 ) (biogenic)) and was in accord with standard hydroxyl radical (OH)-initiated chemistry. Measurement-inferred facility emissions of ethene and propene were far larger than reported by inventories. Substantial direct CH 2 O emissions were not detected from petrochemical facilities. The rapid production of CH 2 O and ozone observed in a highly polluted plume (30+ parts per billion by volume (ppbv) CH 2 O and 200+ ppbv ozone) originating over Houston was well replicated by a model employing only two NMHCs, ethene and propene.
We have measured the rate of reaction of N2O5 with H2O on monodisperse, submicrometer H2SO4 particles in a low‐temperature flow reactor. Measurements were carried out at temperatures between 225 K and 293 K on aerosol particles with sizes and compositions comparable to those found in the stratosphere. At 273 K, the reaction probability was found to be 0.103±0.006, independent of H2SO4 composition from 64 to 81 wt %. At 230 K, the reaction probability increased from 0.077 for compositions near 60% H2S04 to 0.146 for compositions near 70% H2SO4. Intermediate conditions gave intermediate results except for low reaction probabilities of about 0.045 at 260 K on aerosols with about 78% H2SO4. The reaction probability did not depend on particle size. These results imply that the reaction occurs essentially at the surface of the particle. A simple model for this type of reaction that reproduces the general trends observed is presented. The presence of formaldehyde did not affect the reaction rate.
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