Mercury isotopes in a forested ecosystem: Implications for air‐surface exchange dynamics and the global mercury cycle

Forests mediate the biogeochemical cycling of mercury (Hg) between the atmosphere and terrestrial ecosystems; however, there remain many gaps in our understanding of these processes. Our objectives in this study were to characterize Hg isotopic composition within forests, and use natural abundance s...

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Bibliographic Details
Published in:Global Biogeochemical Cycles
Main Authors: Demers, Jason D., Blum, Joel D, Zak, Donald R.
Format: Article in Journal/Newspaper
Language:unknown
Published: Elsevier 2013
Subjects:
Online Access:https://hdl.handle.net/2027.42/97463
https://doi.org/10.1002/gbc.20021
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Summary:Forests mediate the biogeochemical cycling of mercury (Hg) between the atmosphere and terrestrial ecosystems; however, there remain many gaps in our understanding of these processes. Our objectives in this study were to characterize Hg isotopic composition within forests, and use natural abundance stable Hg isotopes to track sources and reveal mechanisms underlying the cycling of Hg. We quantified the stable Hg isotopic composition of foliage, forest floor, mineral soil, precipitation, and total gaseous mercury (THg (g) ) in the atmosphere and in evasion from soil, in 10‐year‐old aspen forests at the Rhinelander FACE experiment in northeastern Wisconsin, USA. The effect of increased atmospheric CO 2 and O 3 concentrations on Hg isotopic composition was small relative to differences among forest ecosystem components. Precipitation samples had δ 202 Hg values of −0.74 to 0.06‰ and ∆ 199 Hg values of 0.16 to 0.82‰. Atmospheric THg (g) had δ 202 Hg values of 0.48 to 0.93‰ and ∆ 199 Hg values of −0.21 to −0.15‰. Uptake of THg (g) by foliage resulted in a large (−2.89‰) shift in δ 202 Hg values; foliage displayed δ 202 Hg values of −2.53 to −1.89‰ and ∆ 199 Hg values of −0.37 to −0.23‰. Forest floor samples had δ 202 Hg values of −1.88 to −1.22‰ and ∆ 199 Hg values of −0.22 to −0.14‰. Mercury isotopes distinguished geogenic sources of Hg and atmospheric derived sources of Hg in soil, and showed that precipitation Hg only accounted for ~16% of atmospheric Hg inputs. The isotopic composition of Hg evasion from the forest floor was similar to atmospheric THg (g) however, there were systematic differences in δ 202 Hg values and MIF of even isotopes (∆ 200 Hg and ∆ 204 Hg). Mercury evasion from the forest floor may have arisen from air‐surface exchange of atmospheric THg (g) , but was not the emission of legacy Hg from soils, nor re‐emission of wet‐deposition. This implies that there was net atmospheric THg (g) deposition to the forest soils. Furthermore, MDF of Hg isotopes during foliar uptake and air‐surface exchange ...