Understanding mercury oxidation and air–snow exchange on the East Antarctic Plateau: a modeling study

摘要

Distinct diurnal and seasonal variations of mercury (Hg) have been observed in near-surface air at Concordia Station on the East Antarctic Plateau, but the processes controlling these characteristics are not well understood. Here, we use a box model to interpret the Hgsup0/sup (gaseous elemental mercury) measurements in thes year 2013. The model includes atmospheric Hgsup0/sup oxidation (by OH, Osub3/sub , or bromine), surface snow HgsupII/sup (oxidized mercury) reduction, and air–snow exchange, and is driven by meteorological fields from a regional climate model. The simulations suggest that a photochemically driven mercury diurnal cycle occurs at the air–snow interface in austral summer. The fast oxidation of Hgsup0/sup in summer may be provided by a two-step bromine-initiated scheme, which is favored by low temperature and high nitrogen oxides at Concordia. The summertime diurnal variations of Hgsup0/sup (peaking during daytime) may be confined within several tens of meters above the snow surface and affected by changing mixed layer depths. Snow re-emission of Hgsup0/sup is mainly driven by photoreduction of snow HgsupII/sup in summer. Intermittent warming events and a hypothesized reduction of HgsupII/sup occurring in snow in the dark may be important processes controlling the mercury variations in the non-summer period, although their relative importance is uncertain. The Br-initiated oxidation of Hgsup0/sup is expected to be slower at Summit Station in Greenland than at Concordia (due to their difference in temperature and levels of nitrogen oxides and ozone), which may contribute to the observed differences in the summertime diurnal variations of Hgsup0/sup between these two polar inland stations.