Abstract
Understanding the distribution and controlling factors of mercury (Hg) speciation in cloud water is crucial for predicting the fate of atmospheric Hg and assessing the environmental impacts of Hg in cloud water. In this study, we collected 85 cloud water samples during autumn and spring at a mountaintop (957 m a.s.l.) in Hong Kong, China. The concentrations of total Hg (THg) in cloud water varied from 3.6 to 225.3 ng L−1, with volume-weighted mean values of 32.1 ng L−1 in autumn and 24.4 ng L−1 in spring. Due to the strong acidic condition of the cloud water, dissolved Hg (DHg) contributed to two-thirds of THg, with Hg complexes by dissolved organic matter (DOM) and chloride being the predominant species of DHg according to chemical equilibrium modeling simulations. Moreover, the levels of Hg-DOM were significantly higher in autumn cloud water compared to spring, and the latter contained more Hg(II)-halide complexes. These differences could be attributed to the different air mass pathways and their emission sources. By combining backward trajectories and Positive Matrix Factorization (PMF) models, we found that air masses originating from the inland Pearl River Delta region, which were only present in autumn cloud water and strongly influenced by stationary coal combustion, were responsible for the highest concentrations of THg, DHg, particulate Hg (PHg) and Hg-DOM. Additionally, air masses originating from regions in China-Indochina Peninsula were only found in spring samples and were significantly influenced by stationary coal combustion, industrial and biogenic sources, contributing to elevated proportions of methylmercury (MeHg) and PHg. In contrast, marine air masses mainly from the western Pacific Ocean contributed to high levels of Hg(II)-halide complexes, especially in spring cloud water. The dissolution and conversion of Hg from sea salt aerosols played a significant role in the enhanced DHg levels observed during cloud processing.
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