Dynamic Surface Interface Exchanges of Mercury: A Review and Compartmentalized Modeling Framework

摘要

This paper presents a review of recent natural surface mercury exchange research in the context of a new modeling framework. The literature indicates that the mercury biogeochemical flux is more dynamic than the current models predict, with interacting multimedia storage and processes. Although several natural mercury emissions models have been created and incorporated into air quality models (AQMs), none are coupled with air quality models on a mass balance basis, and all lack the capacity to explain processes that involve the transport of mercury across atmosphere-surface media concentration gradients. Existing natural mercury emission models treat the surface as both an infinite source and infinite sink for emissions and deposition, respectively,and estimate emissions through the following three pathways: soil, vegetation, and surface waters. The use of these three transport pathways, but with compartmentalized surface storage in a surface-vegetation-atmosphere transport (SVAT) resistance model, is suggested. Surface water fluxes will be modeled using a two-film diffusion model coupled to a surface water photochemical model. This updated framework will allow both the parameterization of the transport of mercury across atmosphere-surface mediaconcentration gradients and the accumulation/depletion of mercury in the surface media. However, several key parameters need further experimental verification before the proposed modeling framework can be implemented in an AQM. These include soil organic mercury interactions, bioavailabil-ity, cuticular transport of mercury, atmospheric surface compensation points for different vegetation species, and enhanced soil diffusion resulting from pressure perturbations.