The influences of ammonia on aerosol formation in the ozonolysis of styrene: roles of Criegee intermediate reactions.

The influences of ammonia (NH) on secondary organic aerosol (SOA) formation from ozonolysis of styrene have been investigated using chamber experiments and quantum chemical calculations. With the value of [O]/[styrene] ratios between 2 and 4, chamber experiments were carried out without NH or under different [NH]/[styrene] ratios. The chamber experiments reveal that the addition of NH led to significant decrease of SOA yield. The overall SOA yield decreased with the [NH]/[styrene] increasing. In addition, the addition of NH at the beginning of the reaction or several hours after the reaction occurs had obviously different influence on the yield of SOA. Gas phase reactions of Criegee intermediates (CIs) with aldehydes and NH were studied in detail by theoretical methods to probe into the mechanisms behind these phenomena. The calculated results showed that 3,5-diphenyl-1,2,4-trioxolane, a secondary ozonide formed through the reactions of CHĊHOO· with CHCHO, could make important contribution to the aerosol composition. The addition of excess NH may compete with aldehydes, decreasing the secondary ozonide yield to some extent and thus affect the SOA formation.