Spatiotemporal distributions and oceanic emissions of short-lived halocarbons in the East China Sea

Abstract

Coastal waters are important sources of volatile halocarbons, which are important in atmospheric chemistry. Here, in May (spring) and October (autumn) 2020, we studied the surface, bottom, and sediment-pore seawater concentrations, atmospheric mixing ratios, and sea-to-air fluxes of the three primary short-lived atmospheric halocarbons (CH3I, CH2Br2, and CHBr3) in the East China Sea (ECS). The highest concentrations of the three short-lived halocarbons occurred in coastal waters, such as the Changjiang estuary and Zhejiang coastal waters, reflecting the influence of excessive anthropogenic inputs on the distributions of these gases. Interestingly, the aqueous levels of these gases seemed to be lower compared to previous measurements in this oceanic region, probably due to reduced contributions from local anthropogenic emission sources. The concentrations of CH3I, CH2Br2, and CHBr3 in pore water were significantly higher than those in bottom water, suggesting that sediment could be a source of these short-lived halocarbons. Additionally, the atmospheric mixing ratios of these gases occasionally increased in coastal areas. An air-mass back trajectory analysis showed this was due to continental anthropogenic sources and emissions from enriched waters. The atmospheric mixing ratios of these halocarbons exhibited significant seasonal variability, with significant correlations among atmospheric CH3I, CH2Br2, and CHBr3 in spring, but not in autumn. The sea-to-air fluxes of CH3I, CH2Br2, and CHBr3 indicated that the ECS is a source of these gases. Seasonal differences in CH3I and CH2Br2 fluxes were driven by changes in wind speed and sea surface temperature, while CHBr3 flux changes were associated with changes in its surface seawater concentration.