skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Unexpected anthropogenic emission decreases explain recent atmospheric mercury concentration declines
Anthropogenic activities emit ~2,000 Mg y−1of the toxic pollutant mercury (Hg) into the atmosphere, leading to long-range transport and deposition to remote ecosystems. Global anthropogenic emission inventories report increases in Northern Hemispheric (NH) Hg emissions during the last three decades, in contradiction with the observed decline in atmospheric Hg concentrations at NH measurement stations. Many factors can obscure the link between anthropogenic emissions and atmospheric Hg concentrations, including trends in the reemissions of previously released anthropogenic (“legacy”) Hg, atmospheric sink variability, and spatial heterogeneity of monitoring data. Here, we assess the observed trends in gaseous elemental mercury (Hg0) in the NH and apply biogeochemical box modeling and chemical transport modeling to understand the trend drivers. Using linear mixed effects modeling of observational data from 51 stations, we find negative Hg0trends in most NH regions, with an overall trend for 2005 to 2020 of −0.011 ± 0.006 ng m−3y−1(±2 SD). In contrast to existing emission inventories, our modeling analysis suggests that annual NH anthropogenic emissions must have declined by at least 140 Mg between the years 2005 and 2020 to be consistent with observed trends. Faster declines in 95th percentile Hg0values than median values in Europe, North America, and East Asian measurement stations corroborate that the likely cause is a decline in nearby anthropogenic emissions rather than background legacy reemissions. Our results are relevant for evaluating the effectiveness of the Minamata Convention on Mercury, demonstrating that existing emission inventories are incompatible with the observed Hg0declines.  more » « less
Award ID(s):
1924148
PAR ID:
10585953
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Proceedings of the National Academy of Sciences
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
121
Issue:
42
ISSN:
0027-8424
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Volcanism is the largest natural source of mercury (Hg) to the biosphere. However, past Hg emission estimates have varied by three orders of magnitude. Here, we present an updated central estimate and interquartile range (232 Mg a−1; IQR: 170–336 Mg a−1) for modern volcanic Hg emissions based on advances in satellite remote sensing of sulfur dioxide (SO2) and an improved method for considering uncertainty in Hg:SO2emissions ratios. Atmospheric modeling shows the influence of volcanic Hg on surface atmospheric concentrations in the extratropical Northern Hemisphere is 1.8 times higher than in the Southern Hemisphere. Spatiotemporal variability in volcanic Hg emissions may obscure atmospheric trends forced by anthropogenic emissions at some locations. This should be considered when selecting monitoring sites to inform global regulatory actions. Volcanic emission estimates from this work suggest the pre‐anthropogenic global atmospheric Hg reservoir was 580 Mg, 7‐fold lower than in 2015 (4,000 Mg). 
    more » « less
  2. Mercury (Hg) is an environmental toxicant dangerous to human health and the environment. Its anthropogenic emissions are regulated by global, regional, and local policies. Here, we investigate Hg sources in the coastal city of Boston, the third largest metropolitan area in the Northeastern United States. With a median of 1.37 ng m −3 , atmospheric Hg concentrations measured from August 2017 to April 2019 were at the low end of the range reported in the Northern Hemisphere and in the range reported at North American rural sites. Despite relatively low ambient Hg concentrations, we estimate anthropogenic emissions to be 3–7 times higher than in current emission inventories using a measurement-model framework, suggesting an underestimation of small point and/or nonpoint emissions. We also test the hypothesis that a legacy Hg source from the ocean contributes to atmospheric Hg concentrations in the study area; legacy emissions (recycling of previously deposited Hg) account for ∼60% of Hg emitted annually worldwide (and much of this recycling takes place through the oceans). We find that elevated concentrations observed during easterly oceanic winds can be fully explained by low wind speeds and recirculating air allowing for accumulation of land-based emissions. This study suggests that the influence of nonpoint land-based emissions may be comparable in size to point sources in some regions and highlights the benefits of further top-down studies in other areas. 
    more » « less
  3. Abstract Mercury (Hg) is a naturally occurring element that has been greatly enriched in the environment by human activities like mining and fossil fuel combustion. Despite commonalities in some carbon dioxide (CO2) and Hg emission sources, the implications of long‐range climate scenarios for anthropogenic Hg emissions have yet to be explored. Here, we present comprehensive projections of anthropogenic Hg emissions extending to the year 2300 and evaluate impacts on global atmospheric Hg deposition. Projections are based on four Shared Socioeconomic Pathways (SSPs) ranging from sustainable reductions in resource and energy intensity to rapid economic growth driven by abundant fossil fuel exploitation. There is a greater than two‐fold difference in cumulative anthropogenic Hg emissions between the lower‐bound (110 Gg) and upper‐bound (235 Gg) scenarios. Hg releases to land and water are approximately six times those of direct emissions to air (600–1,470 Gg). At their peak, anthropogenic Hg emissions reach 2,200–2,600 Mg a−1sometime between 2010 (baseline) and 2030, depending on the SSP scenario. Coal combustion is the largest determinant of differences in Hg emissions among scenarios. Decoupling of Hg and CO2emission sources occurs under low‐to mid‐range scenarios, though contributions from artisanal and small‐scale gold mining remain uncertain. Future Hg emissions may have lower gaseous elemental Hg (Hg0) and higher divalent Hg (HgII), resulting in a higher fraction of locally sourced Hg deposition. Projected reemissions of previously deposited anthropogenic Hg follow a similar temporal trajectory to primary emissions, amplifying the benefits of primary Hg emission reductions under the most stringent mitigation scenarios. 
    more » « less
  4. High levels of methylmercury accumulation in marine biota are a concern throughout the Arctic, where coastal ocean ecosystems received large riverine inputs of mercury (Hg) (40 Mg⋅y −1 ) and sediment (20 Tg⋅y −1 ) during the last decade, primarily from major Russian rivers. Hg concentrations in fish harvested from these rivers have declined since the late 20th century, but no temporal data on riverine Hg, which is often strongly associated with suspended sediments, were previously available. Here, we investigate temporal trends in Russian river particulate Hg (PHg) and total suspended solids (TSS) to better understand recent changes in the Arctic Hg cycle and its potential future trajectories. We used 1,300 measurements of Hg in TSS together with discharge observations made by Russian hydrochemistry and hydrology monitoring programs to examine changes in PHg and TSS concentrations and fluxes in eight major Russian rivers between ca. 1975 and 2010. Due to decreases in both PHg concentrations (micrograms per gram) and TSS loads, annual PHg export declined from 47 to 7 Mg⋅y −1 overall and up to 92% for individual rivers. Modeling of atmospheric Hg deposition together with published inventories on reservoir establishment and industrial Hg release point to decreased pollution and sedimentation within reservoirs as predominant drivers of declining PHg export. We estimate that Russian rivers were the primary source of Hg to the Arctic Ocean in the mid to late 20th century. 
    more » « less
  5. Abstract Soils are a principal global reservoir of mercury (Hg), a neurotoxic pollutant that is accumulating through anthropogenic emissions to the atmosphere and subsequent deposition to terrestrial ecosystems. The fate of Hg in global soils remains uncertain, however, particularly to what degree Hg is re-emitted back to the atmosphere as gaseous elemental mercury (GEM). Here we use fallout radionuclide (FRN) chronometry to directly measure Hg accumulation rates in soils. By comparing these rates with measured atmospheric fluxes in a mass balance approach, we show that representative Arctic, boreal, temperate, and tropical soils are quantitatively efficient at retaining anthropogenic Hg. Potential for significant GEM re-emission appears limited to a minority of coniferous soils, calling into question global models that assume strong re-emission of legacy Hg from soils. FRN chronometry poses a powerful tool to reconstruct terrestrial Hg accumulation across larger spatial scales than previously possible, while offering insights into the susceptibility of Hg mobilization from different soil environments. 
    more » « less