Modelling the mercury stable isotope distribution of Earth surface reservoirs: Implications for global Hg cycling

Sun, Ruoyu and Jiskra, Martin and Amos, Helen M. and Zhang, Yanxu and Sunderland, Elsie M. and Sonke, Jeroen E.. (2019) Modelling the mercury stable isotope distribution of Earth surface reservoirs: Implications for global Hg cycling. Geochimica et Cosmochimica Acta, 246. pp. 156-173.

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Mercury (Hg) stable isotopes are useful to understand Hg biogeochemical cycling because physical, chemical and biological processes cause characteristic Hg isotope mass-dependent (MDF) and mass-independent (MIF) fractionation. Here, source Hg isotope signatures and process-based isotope fractionation factors are integrated into a fully coupled, global atmospheric-terrestrial-oceanic box model of MDF (delta Hg-202), odd-MIF (Delta Hg-199) and even-MIF (Delta Hg-200). Using this bottom-up approach, we find that the simulated Hg isotope compositions are inconsistent with the observations. We then fit the Hg isotope enrichment factors for MDF, odd-MIF and even-MIF to observational Hg isotope constraints. The MDF model suggests that atmospheric Hg-0 photo-oxidation should enrich heavy Hg isotopes in the reactant Hg-0, in contrast to the experimental observations of Hg-0 photo-oxidation by Br. The fitted enrichment factor of terrestrial Hg-0 emission in the odd-MIF model (5 parts per thousand) is likely biased high, suggesting that the terrestrial Hg-0 emission flux (160 Mg yr(-1)) used in our standard model is underestimated. In the even-MIF model, we find that a small positive atmospheric Hg-0 photo-oxidation enrichment factor (0.22 parts per thousand) along with enhanced atmospheric Hg-II photo-reduction and atmospheric Hg-0 dry deposition (foliar uptake) fluxes to the terrestrial reservoir are needed to match Delta Hg-200 observations. Marine Hg isotope measurements are needed to further expand the use of Hg isotopes in understanding global Hg cycling. (C) 2018 Elsevier Ltd. All rights reserved.
Faculties and Departments:05 Faculty of Science > Departement Umweltwissenschaften > Geowissenschaften > Umweltgeowissenschaften (Alewell)
UniBasel Contributors:Jiskra, Martin
Item Type:Article, refereed
Article Subtype:Research Article
Note:Publication type according to Uni Basel Research Database: Journal article
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Last Modified:01 Feb 2021 02:30
Deposited On:08 Jan 2020 07:29

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