Roles of oceanic ventilation and terrestrial outflow in the atmospheric non-methane hydrocarbons over the Chinese marginal seas

Abstract. Non-methane hydrocarbons (NMHCs) in the marine atmosphere have been extensively studied due to their important roles in regulating the atmospheric chemistry and climate. However, very little is known about the distribution and sources of NMHCs in the lower atmosphere over the marginal seas of China. Herein, we characterized the atmospheric NMHCs (C2-C5) in both the coastal cities and marginal seas of China in spring 2021, with a focus on identifying the sources of NMHCs in the coastal atmosphere. The NMHCs in urban atmospheres, especially for alkanes, were significantly higher compared to that in marine atmosphere, suggesting that terrestrial NMHCs may serve as an important reservoir/source of the marine atmosphere. A significant correlation was observed between the alkane concentrations and the distances from sampling sites to the nearest land or retention of air mass over land, indicating that alkanes in the marine atmosphere are largely influenced by terrestrial inputs through air-mass transport. For alkenes, a greater impact from oceanic emissions was determined due to the lower terrestrial concentrations, short atmospheric lifetime, and substantial sea-to-air fluxes of alkenes compared to alkanes (489 ± 454 vs 129 ± 106 nmol m-2 d-1). As suggested by the positive matrix factorization, terrestrial inputs contributed to 89 % of alkanes and 69.6 % of alkenes in Chinese marginal seas, subsequently contributing to 84 % of the ozone formation potential associated with C2-C5 NMHCs. These findings underscore the significance of terrestrial outflow in controlling the distribution and composition of atmospheric NMHCs in the marginal seas of China.