Mass-dependent fractionation (MDF) and mass-independent fractionation (MIF) of Hg isotopes provides a new tool for tracing Hg in contaminated environments such as mining sites, which represent major point sources of Hg pollution into surrounding ecosystems. Here, we present Hg isotope ratios of unroasted ore waste, calcine (roasted ore), and poplar leaves collected at a closed Hg mine (New Idria, CA, U.S.A.). Unroasted ore waste was isotopically uniform with δ(202)Hg values from -0.09 to 0.16‰ (± 0.10‰, 2 SD), close to the estimated initial composition of the HgS ore (-0.26‰). In contrast, calcine samples exhibited variable δ(202)Hg values ranging from -1.91‰ to +2.10‰. Small MIF signatures in the calcine were consistent with nuclear volume fractionation of Hg isotopes during or after the roasting process. The poplar leaves exhibited negative MDF (-3.18 to -1.22‰) and small positive MIF values (Δ(199)Hg of 0.02 to 0.21‰). Sequential extractions combined with Hg isotope analysis revealed higher δ(202)Hg values for the more soluble Hg pools in calcines compared with residual HgS phases. Our data provide novel insights into possible in situ transformations of Hg phases and suggest that isotopically heavy secondary Hg phases were formed in the calcine, which will influence the isotope composition of Hg leached from the site.
Better understanding of mercury (Hg) accumulation, distribution, and speciation in plants is required to evaluate potential risks for the environment and to optimize phytostabilization strategies for Hg-contaminated soils. The behavior of Hg in alfalfa (Medicago sativa) plants grown under controlled conditions in a hydroponic system (30 μM HgCl2) was compared with that of naturally occurring Horehound (Marrubium vulgare) plants collected from a mining soil polluted with Hg (Almadenejos, Spain) to characterize common mechanisms of tolerance. Synchrotron X-ray Fluorescence microprobe (μ-SXRF) showed that Hg accumulated at the root apex of alfalfa and was distributed through the vascular system to the leaves. Transmission electron microscopy (TEM) implied association of Hg with cell walls, accompanied by their structural changes, in alfalfa roots. Extended X-ray absorption fine structure (EXAFS) determined that Hg was principally bound to biothiols and/or proteins in M. sativa roots, stems, and leaves. However, the major fraction of Hg detected in M. vulgare plants consisted of mineral species, possibly associated with soil components. Interestingly, the fraction of Hg bound to biothiols/proteins (i.e., metabolically processed Hg) in leaves of both plants (alfalfa and M. vulgare) was similar, in spite of the big difference in Hg accumulation in roots, suggesting that some tolerance mechanisms might be shared.
The spreading of reverse-osmosis desalinated seawater (DSW) in the Israeli coastal aquifer was studied using groundwater modeling and stable water isotopes as tracers. The DSW produced at the Hadera seawater reverse-osmosis (SWRO) desalination plant is recharged into the aquifer through an infiltration pond at the managed aquifer recharge (MAR) site of Menashe, Israel. The distinct difference in isotope composition between DSW (δ 18 O = 1.41 ‰; δ 2 H = 11.34 ‰) and the natural groundwater (δ 18 O = −4.48 ‰ to −5.43 ‰; δ 2 H = −18.41 ‰ to −22.68 ‰) makes the water isotopes preferable for use as a tracer compared to widely used chemical tracers, such as chloride. Moreover, this distinct difference can be used to simplify the system to a binary mixture of two end-members: desalinated seawater and groundwater. This approach is validated through a sensitivity analysis, and it is especially robust when spatial data of stable water isotopes in the aquifer are scarce. A calibrated groundwater flow and transport model was used to predict the DSW plume distribution in the aquifer after 50 years of MAR with DSW. The results suggest that after 50 years, 94 % of the recharged DSW was recovered by the production wells at the Menashe MAR site. The presented methodology is useful for predicting the distribution of reverse-osmosis desalinated seawater in various downstream groundwater systems.
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