The reaction of Criegee intermediates with formamide and its implication to atmospheric aerosols

The reactions of Criegee intermediates (CIs) play an important role in the formation of secondary organic aerosols that have negative effect on visibility, human health, and global climate. New particle formation (NPF) can contribute to more than half of the aerosols in terms of their number concentration. Here, the reactions of CIs with formamide (FA) in the gas-phase and at the air/water interface were investigated using quantum chemistry calculation and Born-Oppenheimer molecular dynamic simulations. The results show that the reaction mechanism of CIs with FA is similar to that with formic acid, and the formation of hydroperoxymethyl formimidate (P4) is the most favorable pathway both in the gas-phase and at the air/water interface. Moreover, the potential contribution of the products to NPF was also evaluated by means of the molecular dynamic simulations. The results indicate that the product (P4) can participate in the SA-based NPF and water molecules are beneficial to enhance the NPF. The exploration will provide insight into the reaction of CIs with amide and the effect of the Criegee chemistry on the atmospheric aerosols.