Legacy Mercury Re-emission and Subsurface Migration at Contaminated Sites Constrained by Hg Isotopes and Chemical Speciation
The re-emission and subsurface migration of legacy mercury (Hg) are not well understood due to limited knowledge of the driving processes. To investigate these processes at a decommissioned chlor-alkali plant, we used mercury stable isotopes and chemical speciation analysis. The isotopic composition of volatilized Hg(0) was lighter compared to the bulk total Hg (THg) pool in salt-sludge and adjacent surface soil with mean ε202HgHg(0)-THg values of -3.29 and -2.35‰, respectively. Hg(0) exhibited dichotomous directions (E199HgHg(0)-THg = 0.17 and -0.16‰) of mass-independent fractionation (MIF) depending on the substrate from which it was emitted. We suggest that the positive MIF enrichment during Hg(0) re-emission from salt-sludge was overall controlled by the photoreduction of Hg(II) primarily ligated by Cl- and/or the evaporation of liquid Hg(0). In contrast, O-bonded Hg(II) species were more important in the adjacent surface soils. The migration of Hg from salt-sludge to subsurface soil associated with selective Hg(II) partitioning and speciation transformation resulted in deep soils depleted in heavy isotopes (δ202Hg = -2.5‰) and slightly enriched in odd isotopes (Δ199Hg = 0.1‰). When tracing sources using Hg isotopes, it is important to exercise caution, particularly when dealing with mobilized Hg, as this fraction represents only a small portion of the sources.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:58 |
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| Enthalten in: |
Environmental science & technology - 58(2024), 12 vom: 26. März, Seite 5336-5346 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Zhu, Wei [VerfasserIn] |
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| Links: |
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| Themen: |
FXS1BY2PGL |
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| Anmerkungen: |
Date Completed 27.03.2024 Date Revised 30.03.2024 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/acs.est.3c07276 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM369618076 |
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| 520 | |a The re-emission and subsurface migration of legacy mercury (Hg) are not well understood due to limited knowledge of the driving processes. To investigate these processes at a decommissioned chlor-alkali plant, we used mercury stable isotopes and chemical speciation analysis. The isotopic composition of volatilized Hg(0) was lighter compared to the bulk total Hg (THg) pool in salt-sludge and adjacent surface soil with mean ε202HgHg(0)-THg values of -3.29 and -2.35‰, respectively. Hg(0) exhibited dichotomous directions (E199HgHg(0)-THg = 0.17 and -0.16‰) of mass-independent fractionation (MIF) depending on the substrate from which it was emitted. We suggest that the positive MIF enrichment during Hg(0) re-emission from salt-sludge was overall controlled by the photoreduction of Hg(II) primarily ligated by Cl- and/or the evaporation of liquid Hg(0). In contrast, O-bonded Hg(II) species were more important in the adjacent surface soils. The migration of Hg from salt-sludge to subsurface soil associated with selective Hg(II) partitioning and speciation transformation resulted in deep soils depleted in heavy isotopes (δ202Hg = -2.5‰) and slightly enriched in odd isotopes (Δ199Hg = 0.1‰). When tracing sources using Hg isotopes, it is important to exercise caution, particularly when dealing with mobilized Hg, as this fraction represents only a small portion of the sources | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Hg contaminated sites | |
| 650 | 4 | |a Hg isotope fractionation | |
| 650 | 4 | |a Hg speciation | |
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| 700 | 1 | |a Li, Zhonggen |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Ping |e verfasserin |4 aut | |
| 700 | 1 | |a Sommar, Jonas |e verfasserin |4 aut | |
| 700 | 1 | |a Fu, Xuewu |e verfasserin |4 aut | |
| 700 | 1 | |a Feng, Xinbin |e verfasserin |4 aut | |
| 700 | 1 | |a Yu, Ben |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Reis, Ana T |e verfasserin |4 aut | |
| 700 | 1 | |a Pereira, Eduarda |e verfasserin |4 aut | |
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