We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg-0 observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg-0 and wet deposition measurements. The optimized global mercury emission to the atmosphere is 5.8 Gg yr(-1). The ocean accounts for 3.2 Gg yr(-1) (55 % of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg-0. The optimized Asian anthropogenic emission of Hg-0 (gas elemental mercury) is 650-1770 Mg yr(-1), higher than its bottom-up estimates (550-800 Mg yr(-1)). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition

No abstract

No abstract

Dry deposition fluxes and deposition velocities (=deposition flux/atmospheric concentration) for trace metals including Hg, Cd, Cu, Mn, Pb, and Zn in the Tokyo metropolitan area were measured using an improved water surface sampler. Mercury is deposited on the water surface in both gaseous (reactive gaseous mercury, RGM) and particulate (particulate mercury, Hg(p)) forms. The results based on 1 yr observations found that dry deposition plays a significant if not dominant role in trace metal deposition in this urban area, contributing fluxes ranging from 0.46 (Cd) to 3.0 (Zn) times those of concurrent wet deposition fluxes. The deposition velocities were found to be dependent on the deposition of coarse particles larger than approximately 5 microm in diameter on the basis of model calculations. Our analysis suggests that the 84.13% diameter is a more appropriate index for each deposited metal than the 50% diameter in the assumed undersize log-normal distribution, because larger particles are responsible for the flux. The deposition velocities for trace metals other than mercury increased exponentially with an increase in their 84.13% diameters. Using this regression equation, the deposition velocities for Hg(p) were estimated from its 84.13% diameter. The deposition fluxes for Hg(p) calculated from the estimated velocities tended to be close to the mercury fluxes measured with the water surface sampler during the study periods except during summer.

Abstract. We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physio-chemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg0 observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations, and also matches regional over-water Hg0 and wet deposition measurements. The optimized global mercury emission to the atmosphere is ~5.8 Gg yr−1. The ocean accounts for 3.2 Gg yr−1 (55% of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg0. The optimized Asian anthropogenic emission of Hg0 (gas elemental mercury) is 650–1770 Mg yr−1, higher than its bottom-up estimates (550–800 Mg yr−1). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23% of present-day atmospheric deposition.