Twenty years of studying the origins and fate of atmospheric mercury over the Mediterranean Sea.

This study provides a review of 13 oceanographic campaigns between 2000 and 2017 to measure Hg in the Mediterranean, highlighting major findings from measurement and modelling activities during the Med-Oceanor program. The initial campaigns showed that high concentrations of RGM could be found far from industrial source regions and the observed daily variation in concentration, with peaks at midday and lower concentrations during darkness gave the first indications that photochemically mediated oxidation reactions were producing RGM in the MBL. Later atmospheric chemistry modelling studies showed the feasibility of Hg oxidation by bromine containing oxidants, which are released as a result of the acidification of sea salt aerosols in the Marine Boundary Layer (MBL). Spatial and seasonal variations of DGM were observed at different depths in the water column, with average DGM concentrations higher in the West and East Mediterranean deep and intermediate waters, than in overlaying Atlantic waters. DGM in water profiles typically increased with depth, together with nutrients and decreasing oxygen, indicating a possible bacterial and/or geogenic origin. Using measured DGM and meteorological variable values Hg fluxes can be calculated. When these are included in regional and global models they suggest that the net Hg evasion from the Mediterranean is around 30 Mg yr. Repetition of these campaigns should be an extremely high priority, both to continue to monitor changes in atmospheric and aquatic Hg species concentrations, but also to perform RGM detection methodology intercomparisons so that the historical data is adequately contextualised and may be used to evaluate temporal trends.