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SO 2 oxidation and nucleation studies at near-atmospheric conditions in outdoor smog chamber

SO 2 oxidation and nucleation studies at near-atmospheric conditions in outdoor smog chamber Environmental context Nucleation, a fundamental step in atmospheric new-particle formation, is a significant source of atmospheric aerosols. Most laboratory experiments investigate H 2 SO 4 nucleation based on indoor chambers or flow tube reactors, and find discrepancies with field observations. Here a large outdoor smog chamber is used to study the relationship between SO 2 and nucleation rates, and demonstrate the importance of aqueous phase oxidation of SO 2 by H 2 O 2 and other oxidants. Abstract Particle formation under different initial ambient background conditions was simulated in a dual outdoor smog chamber for the SO 2 and O 3 –SO 2 systems with and without sunlight, as well as a propylene–NO x –SO 2 –sunlight system. An exponential power of 1.37 between nucleation rates at 1 nm ( J 1 ) and SO 2 gas phase concentrations was obtained for the SO 2 –sunlight system and a minimum of 0.45 ppb SO 2 is required by this relationship to initiate nucleation ( J 1 is equal to 1 cm –3 s –1 ). An investigation of the O 3 –SO 2 –sunlight/dark system showed that the presence of O 3 contributed to the particle nucleation and growth at night; however, it only enhanced the particle growth in the daytime when H 2 SO 4 photochemistry was present. In the presence of an OH • scavenger, the O 3 –SO 2 system did not show particle nucleation, suggesting that the scavenger cut off this pathway of SO 2 oxidation. A lower nucleation rate and higher particle grow rate were also observed for SO 2 oxidation in the presence of propylene and NO x . However a higher SO 2 decay rate was obtained for the propylene system especially under high relative humidity, which was not observed in the O 3 –SO 2 system. This suggests that aqueous phase oxidation of SO 2 from H 2 O 2 , RO 2 • and other oxidants produced in the propylene–NO x system contribute to the particle growth. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Environmental Chemistry CSIRO Publishing

SO 2 oxidation and nucleation studies at near-atmospheric conditions in outdoor smog chamber

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Publisher
CSIRO Publishing
Copyright
CSIRO
ISSN
1448-2517
eISSN
1449-8979
DOI
10.1071/EN13024
Publisher site
See Article on Publisher Site

Abstract

Environmental context Nucleation, a fundamental step in atmospheric new-particle formation, is a significant source of atmospheric aerosols. Most laboratory experiments investigate H 2 SO 4 nucleation based on indoor chambers or flow tube reactors, and find discrepancies with field observations. Here a large outdoor smog chamber is used to study the relationship between SO 2 and nucleation rates, and demonstrate the importance of aqueous phase oxidation of SO 2 by H 2 O 2 and other oxidants. Abstract Particle formation under different initial ambient background conditions was simulated in a dual outdoor smog chamber for the SO 2 and O 3 –SO 2 systems with and without sunlight, as well as a propylene–NO x –SO 2 –sunlight system. An exponential power of 1.37 between nucleation rates at 1 nm ( J 1 ) and SO 2 gas phase concentrations was obtained for the SO 2 –sunlight system and a minimum of 0.45 ppb SO 2 is required by this relationship to initiate nucleation ( J 1 is equal to 1 cm –3 s –1 ). An investigation of the O 3 –SO 2 –sunlight/dark system showed that the presence of O 3 contributed to the particle nucleation and growth at night; however, it only enhanced the particle growth in the daytime when H 2 SO 4 photochemistry was present. In the presence of an OH • scavenger, the O 3 –SO 2 system did not show particle nucleation, suggesting that the scavenger cut off this pathway of SO 2 oxidation. A lower nucleation rate and higher particle grow rate were also observed for SO 2 oxidation in the presence of propylene and NO x . However a higher SO 2 decay rate was obtained for the propylene system especially under high relative humidity, which was not observed in the O 3 –SO 2 system. This suggests that aqueous phase oxidation of SO 2 from H 2 O 2 , RO 2 • and other oxidants produced in the propylene–NO x system contribute to the particle growth.

Journal

Environmental Chemistry – CSIRO Publishing

Published: Jun 28, 2013

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