Mercury transport, transformation and mass balance on a perspective of hydrological processes in a subtropical forest of China

Forest ecosystem has long been suggested as a vital component in the global mercury (Hg) biogeochemical cycling. However, there remains large uncertainties in understanding total Hg (THg) and methylmercury (MeHg) variations and their controlling factors during the whole hydrological processes in forest ecosystems. Here, we quantified Hg mass flow along hydrological processes of wet deposition, throughfall, stemflow, litter leachate, soil leachate, surface runoff, and stream, and litterfall Hg deposition, and air-forest floor elemental Hg (Hg⁰) exchange flux to set up a Hg mass balance in a subtropical forest of China. Results showed that THg concentration in stream was lower than that in wet deposition, while an opposite characteristic for MeHg concentration, and both THg and MeHg fluxes of stream were lower than those of wet deposition. Variations of THg and MeHg in throughfall and litter leachate had strong direct and indirect effects on controlling variations of THg and MeHg in surface runoff, soil leachate and stream, respectively. Especially, the net Hg methylation was suggested in the forest canopy and forest floor layers, and significant particulate bound Hg (PBM) filtration was observed in soil layers. The Hg mass balance showed that the litterfall Hg deposition was the main Hg input for forest floor Hg, and the elemental Hg vapor (Hg⁰) re-emission from forest floor was the dominant Hg output. Overall, we estimated the net THg input flux of 13.8 μg m⁻² yr⁻¹ and net MeHg input flux of 0.6 μg m⁻² yr⁻¹ within the forest ecosystem. Our results highlighted the important roles of forest canopy and forest floor to shape Hg in output flow, and the forest floor is a distinct sink of MeHg.