A review of global environmental mercury processes in response to human and natural perturbations: Changes of emissions, climate, and land use

We review recent progress in our understanding of the global cycling of mercury (Hg), including best estimates of Hg concentrations and pool sizes in major environmental compartments and exchange processes within and between these reservoirs. Recent advances include the availability of new global datasets covering areas of the world where environmental Hg data were previously lacking; integration of these data into global and regional models is continually improving estimates of global Hg cycling. New analytical techniques, such as Hg stable isotope characterization, provide novel constraints of sources and transformation processes. The major global Hg reservoirs that are, and continue to be, affected by anthropogenic activities include the atmosphere (4.4–5.3 Gt), terrestrial environments (particularly soils: 250–1000 Gg), and aquatic ecosystems (e.g., oceans: 270–450 Gg). Declines in anthropogenic Hg emissions between 1990 and 2010 have led to declines in atmospheric Hg[superscript 0] concentrations and Hg[supercript II] wet deposition in Europe and the US (− 1.5 to − 2.2% per year). Smaller atmospheric Hg[superscript 0] declines (− 0.2% per year) have been reported in high northern latitudes, but not in the southern hemisphere, while increasing atmospheric Hg loads are still reported in East Asia. New observations and updated models now suggest high concentrations of oxidized Hg[superscript II] in the tropical and subtropical free troposphere where deep convection can scavenge these Hg[superscript II] reservoirs. As a result, up to 50% of total global wet Hg[superscript II] deposition has been predicted to occur to tropical oceans. Ocean Hg[superscript 0] evasion is a large source of present-day atmospheric Hg (approximately 2900 Mg/year; range 1900–4200 Mg/year). Enhanced seawater Hg[superscript 0] levels suggest enhanced Hg[superscript 0] ocean evasion in the intertropical convergence zone, which may be linked to high HgII deposition. Estimates of gaseous Hg[superscript 0] emissions to the atmosphere over land, long considered a critical Hg source, have been revised downward, and most terrestrial environments now are considered net sinks of atmospheric Hg due to substantial Hg uptake by plants. Litterfall deposition by plants is now estimated at 1020–1230 Mg/year globally. Stable isotope analysis and direct flux measurements provide evidence that in many ecosystems Hg0 deposition via plant inputs dominates, accounting for 57–94% of Hg in soils. Of global aquatic Hg releases, around 50% are estimated to occur in China and India, where Hg drains into the West Pacific and North Indian Oceans. A first inventory of global freshwater Hg suggests that inland freshwater Hg releases may be dominated by artisanal and small-scale gold mining (ASGM; approximately 880 Mg/year), industrial and wastewater releases (220 Mg/year), and terrestrial mobilization (170–300 Mg/year). For pelagic ocean regions, the dominant source of Hg is atmospheric deposition; an exception is the Arctic Ocean, where riverine and coastal erosion is likely the dominant source. Ocean water Hg concentrations in the North Atlantic appear to have declined during the last several decades but have increased since the mid-1980s in the Pacific due to enhanced atmospheric deposition from the Asian continent. Finally, we provide examples of ongoing and anticipated changes in Hg cycling due to emission, climate, and land use changes. It is anticipated that future emissions changes will be strongly dependent on ASGM, as well as energy use scenarios and technology requirements implemented under the Minamata Convention. We predict that land use and climate change impacts on Hg cycling will be large and inherently linked to changes in ecosystem function and global atmospheric and ocean circulations. Our ability to predict multiple and simultaneous changes in future Hg global cycling and human exposure is rapidly developing but requires further enhancement. Keywords: Climate change, Emission change, Heavy metal, Land use change, Mercury global environmental cyclingNational Institute of Environmental Health Sciences (Dartmouth College. Toxic Metals Superfund Research Program. Award R13 ES028077-01)National Institute of Environmental Health Sciences (Dartmouth College. Toxic Metals Superfund Research Program. Award P42ES007373)National Science Foundation (U.S.) (CNH 1313755)Horizon 2020 Framework Programme (European Commission) (Marie Sklodowska-Curie Grant Agreement 657195)National Science Foundation (U.S.) (PLR 1304305