Unveiling the overlooked direct emissions of particulate organic nitrates from ship.

ABSTRACT

Particulate organic nitrates (pONs) have drawn growing interests due to their effects on nitrogen cycling, air pollution, and regional climate. While secondary formation is typically considered as the major source of pONs, direct emissions from various sources remain poorly explored. Ship exhausts have been known as an important source of reactive nitrogen species, yet pONs emissions from ship have been rarely characterized. In this study, we conducted atmospheric measurement of pONs during a ship-based cruise measurement campaign in the East China Sea and also emission measurement of pONs from ship exhausts. During the ship-based cruise, total five typical kinds of pONs were determined and the average total concentrations of five pONs were 479 ± 193 and 250 ± 139 ng m-3 when sampling was influenced by ship emissions or not, respectively, indicating the notable impact of ship exhaust plumes on ambient pONs. Further, five typical pONs were successfully identified and quantified from ship exhausts, with the average total concentration of 1123 ± 406 µg m-3. The much higher pONs levels in ship exhausts than in ambient particulate matters demonstrated ship emission as an important source for pONs. Additionally, their emission factors from ship exhausts were determined as at a range of 0.1-12.6 mg kWh-1. The chemical transport model simulations indicate that direct pONs emissions from ship exert a significant contribution to atmospheric pONs, especially in the clean marine atmosphere. These findings provide compelling evidence for direct emission of pONs from ship and its considerable effects. We call for further studies to better characterize the direct pONs emissions from ship and other potential sources, which should be incorporated into global and regional models.