SO2 oxidation and nucleation studies at near-atmospheric conditions in outdoor smog chamber
Yang Zhou A B C , Elias P. Rosen B E G , Haofei Zhang B F , Weruka Rattanavaraha B , Wenxing Wang A D and Richard M. Kamens B
+ Author Affiliations
- Author Affiliations
A Environment Research Institute, Shandong University, Jinan, 250100, China.
B Department of Environmental Science and Engineering, University of North Carolina, Chapel Hill, NC 27599, USA.
C Division of Environment, The Hong Kong University of Science &Technology, Clear Water Bay, Kowloon, Hong Kong, China.
D Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
E Present address: Southwest Sciences, Inc., 1570 Pacheco Street, Suite E-11 Santa Fe, NM 87505, USA.
F Present address: Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
G Corresponding author. Email: elirosen@gmail.com
Environmental Chemistry 10(3) 210-220 https://doi.org/10.1071/EN13024
Submitted: 31 January 2013 Accepted: 14 May 2013 Published: 28 June 2013
Environmental context. Nucleation, a fundamental step in atmospheric new-particle formation, is a significant source of atmospheric aerosols. Most laboratory experiments investigate H2SO4 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 SO2 and nucleation rates, and demonstrate the importance of aqueous phase oxidation of SO2 by H2O2 and other oxidants.
Abstract. Particle formation under different initial ambient background conditions was simulated in a dual outdoor smog chamber for the SO2 and O3–SO2 systems with and without sunlight, as well as a propylene–NOx–SO2–sunlight system. An exponential power of 1.37 between nucleation rates at 1 nm (J1) and SO2 gas phase concentrations was obtained for the SO2–sunlight system and a minimum of 0.45 ppb SO2 is required by this relationship to initiate nucleation (J1 is equal to 1 cm–3 s–1). An investigation of the O3–SO2–sunlight/dark system showed that the presence of O3 contributed to the particle nucleation and growth at night; however, it only enhanced the particle growth in the daytime when H2SO4 photochemistry was present. In the presence of an OH• scavenger, the O3–SO2 system did not show particle nucleation, suggesting that the scavenger cut off this pathway of SO2 oxidation. A lower nucleation rate and higher particle grow rate were also observed for SO2 oxidation in the presence of propylene and NOx. However a higher SO2 decay rate was obtained for the propylene system especially under high relative humidity, which was not observed in the O3–SO2 system. This suggests that aqueous phase oxidation of SO2 from H2O2, RO2• and other oxidants produced in the propylene–NOx system contribute to the particle growth.
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