Isotopic composition of total gaseous mercury at a high-altitude tropical forest site influenced by air masses from the East Asia continent and the Pacific Ocean

Abstract

Gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), particulate-bound mercury (PBM), and the isotopic composition of total gaseous mercury (TGM = GEM + GOM) were measured at the Lulin Atmospheric Background Station (LABS), a mountain background site downwind of the East Asia continent, from February 2015 to January 2016. Mean (±S.D.) concentrations of GEM, GOM, and PBM were 1.54 ± 0.34 ng m−3, 14.0 ± 27.8 pg m−3, and 2.6 ± 3.7 pg m−3, respectively. Concentration-Weighted Trajectory (CWT) analysis indicated that East and coastal China were the main source regions of elevated GEM observed at LABS. Weekly integrated TGM showed significant variations in δ202HgTGM (−0.42 to 0.41‰) and Δ199HgTGM (−0.31 to −0.13‰). Both δ202HgTGM and Δ199HgTGM showed clear seasonal variations, but the seasonal pattern of δ202HgTGM was different from that of Δ199HgTGM. The lowest mean δ202HgTGM was observed in spring (−0.15‰), while the lowest mean Δ199HgTGM was observed in summer (−0.24‰). A significant positive correlation (R2 = 0.38, p < 0.01) existed between δ202HgTGM and normalized difference vegetation index (NDVI), suggesting vegetation activity was an important factor controlling the seasonal variation of δ202HgTGM. In contrast, air mass transport path, which influences the source region of TGM to LABS, was likely the driver for the seasonal variations of Δ199HgTGM. Furthermore, results from the air mass classification showed distinguishable Δ199HgTGM signature for different air mass source regions, with air masses from South China Sea and western Pacific Ocean being characterized by more negative Δ199HgTGM (−0.25 ± 0.04‰). Results of this research demonstrated a clear difference in isotopic compositions of atmospheric Hg between continental and marine air masses.