Spatial patterns of Zn, Cd, and Pb isotopic compositions of ground and surface water in mine areas of South Korea reflecting isotopic fractionation during metal attenuation

Duk Min Kim; Man Sik Choi; Seong Taek Yun; Sungmoon Yoon; Jin Soo Lee

doi:10.1016/j.scitotenv.2021.146453

Spatial patterns of Zn, Cd, and Pb isotopic compositions of ground and surface water in mine areas of South Korea reflecting isotopic fractionation during metal attenuation

Duk Min Kim, Man Sik Choi, Seong Taek Yun, Sungmoon Yoon, Jin Soo Lee

Department of Earth and Environmental Sciences

Research output: Contribution to journal › Article › peer-review

8 Citations (Scopus)

Abstract

As application of multiple metal isotopes can effectively constrain geochemical behavior of contaminants and assess contamination sources and pathways, field-scale studies on the geochemically interlinked fractionation of Zn and Cd isotopes in groundwater are needed. In this study, we collected groundwater samples from multi-level samplers downstream of tailings dumps as well as surface water, ore mineral, precipitate, and tailings samples at the Sambo and Buddeun metallic ore mines in South Korea, and analyzed their Zn, Cd, Pb, and sulfur isotopic compositions. Furthermore, isotopic ratios of ore mineral samples from additional four mines in South Korea (Dangdu, Dongbo, Gomyeong, Samgwang) were compared. A dual isotopic approach using Zn and Cd isotopes was used to assess fractionation processes, and Pb isotopic signatures reflecting their sources were assessed. Increasing trends of δ⁶⁶Zn and δ¹¹⁴Cd with decreasing Zn and Cd concentrations were observed in groundwater, which was saturated with respect to ZnS (amorphous and sphalerite) and CdS (greenockite). Moreover, for some groundwater samples, δ⁶⁶Zn showed a positive relationship with δ³⁴S_SO4. These results suggest that Zn and Cd are precipitated as sulfide following sulfate reduction. In the plot of δ⁶⁶Zn against δ¹¹⁴Cd, relatively high and/or increasing δ⁶⁶Zn in groundwater suggested the effect of fractionation due to sulfide precipitation, while variable and high δ¹¹⁴Cd values suggested the fractionation by adsorption and/or sulfide precipitation, which were based on positive fractionation factors for δ⁶⁶Zn and δ¹¹⁴Cd during sulfide precipitation and mostly negative and positive fractionation factors for δ⁶⁶Zn and δ¹¹⁴Cd, respectively, during adsorption. This study shows that the combined use of Zn and Cd isotopes in groundwater can effectively differentiate between adsorption and sulfide precipitation following sulfate reduction in groundwater. Additionally, the ²⁰⁸Pb/²⁰⁶Pb ratios of most water samples reflected those of ore and tailings samples, which verified usefulness of Pb isotopes in water in investigating Pb contamination sources.

Original language	English
Article number	146453
Journal	Science of the Total Environment
Volume	779
DOIs	https://doi.org/10.1016/j.scitotenv.2021.146453
Publication status	Published - 2021 Jul 20

Bibliographical note

Funding Information:
This work was initially supported by a research fund (to S.T. Yun) from the Korea Mine Reclamation Corporation (MIRECO) funded by the Ministry of Trade, Industry, and Energy . Students at the Chemical Oceanography Laboratory in Chungnam University and at the Environmental Geochemistry Laboratory in Korea University, as well as Ji-Hye Hong at MIRECO, assisted the authors with well installation, field work, and data preparation. The completion of this work was partially supported by the Korea Environmental Industry & Technology Institute (KEITI) through the Subsurface Environment Management (SEM) Project, funded by the Korea Ministry of Environment (MOE). Special thanks go to four anonymous reviewers for providing critical and constructive comments and suggestions that helped to significantly improve the manuscript.

Publisher Copyright:
© 2021 Elsevier B.V.

Keywords

Adsorption
Fractionation
Mining area
Sulfide precipitation
Zn and Cd isotopes

ASJC Scopus subject areas

Environmental Engineering
Environmental Chemistry
Waste Management and Disposal
Pollution

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10.1016/j.scitotenv.2021.146453

Cite this

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title = "Spatial patterns of Zn, Cd, and Pb isotopic compositions of ground and surface water in mine areas of South Korea reflecting isotopic fractionation during metal attenuation",

abstract = "As application of multiple metal isotopes can effectively constrain geochemical behavior of contaminants and assess contamination sources and pathways, field-scale studies on the geochemically interlinked fractionation of Zn and Cd isotopes in groundwater are needed. In this study, we collected groundwater samples from multi-level samplers downstream of tailings dumps as well as surface water, ore mineral, precipitate, and tailings samples at the Sambo and Buddeun metallic ore mines in South Korea, and analyzed their Zn, Cd, Pb, and sulfur isotopic compositions. Furthermore, isotopic ratios of ore mineral samples from additional four mines in South Korea (Dangdu, Dongbo, Gomyeong, Samgwang) were compared. A dual isotopic approach using Zn and Cd isotopes was used to assess fractionation processes, and Pb isotopic signatures reflecting their sources were assessed. Increasing trends of δ66Zn and δ114Cd with decreasing Zn and Cd concentrations were observed in groundwater, which was saturated with respect to ZnS (amorphous and sphalerite) and CdS (greenockite). Moreover, for some groundwater samples, δ66Zn showed a positive relationship with δ34SSO4. These results suggest that Zn and Cd are precipitated as sulfide following sulfate reduction. In the plot of δ66Zn against δ114Cd, relatively high and/or increasing δ66Zn in groundwater suggested the effect of fractionation due to sulfide precipitation, while variable and high δ114Cd values suggested the fractionation by adsorption and/or sulfide precipitation, which were based on positive fractionation factors for δ66Zn and δ114Cd during sulfide precipitation and mostly negative and positive fractionation factors for δ66Zn and δ114Cd, respectively, during adsorption. This study shows that the combined use of Zn and Cd isotopes in groundwater can effectively differentiate between adsorption and sulfide precipitation following sulfate reduction in groundwater. Additionally, the 208Pb/206Pb ratios of most water samples reflected those of ore and tailings samples, which verified usefulness of Pb isotopes in water in investigating Pb contamination sources.",

keywords = "Adsorption, Fractionation, Mining area, Sulfide precipitation, Zn and Cd isotopes",

author = "Kim, {Duk Min} and Choi, {Man Sik} and Yun, {Seong Taek} and Sungmoon Yoon and Lee, {Jin Soo}",

note = "Funding Information: This work was initially supported by a research fund (to S.T. Yun) from the Korea Mine Reclamation Corporation (MIRECO) funded by the Ministry of Trade, Industry, and Energy . Students at the Chemical Oceanography Laboratory in Chungnam University and at the Environmental Geochemistry Laboratory in Korea University, as well as Ji-Hye Hong at MIRECO, assisted the authors with well installation, field work, and data preparation. The completion of this work was partially supported by the Korea Environmental Industry & Technology Institute (KEITI) through the Subsurface Environment Management (SEM) Project, funded by the Korea Ministry of Environment (MOE). Special thanks go to four anonymous reviewers for providing critical and constructive comments and suggestions that helped to significantly improve the manuscript. Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

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doi = "10.1016/j.scitotenv.2021.146453",

language = "English",

volume = "779",

journal = "Science of the Total Environment",

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T1 - Spatial patterns of Zn, Cd, and Pb isotopic compositions of ground and surface water in mine areas of South Korea reflecting isotopic fractionation during metal attenuation

AU - Kim, Duk Min

AU - Choi, Man Sik

AU - Yun, Seong Taek

AU - Yoon, Sungmoon

AU - Lee, Jin Soo

N1 - Funding Information: This work was initially supported by a research fund (to S.T. Yun) from the Korea Mine Reclamation Corporation (MIRECO) funded by the Ministry of Trade, Industry, and Energy . Students at the Chemical Oceanography Laboratory in Chungnam University and at the Environmental Geochemistry Laboratory in Korea University, as well as Ji-Hye Hong at MIRECO, assisted the authors with well installation, field work, and data preparation. The completion of this work was partially supported by the Korea Environmental Industry & Technology Institute (KEITI) through the Subsurface Environment Management (SEM) Project, funded by the Korea Ministry of Environment (MOE). Special thanks go to four anonymous reviewers for providing critical and constructive comments and suggestions that helped to significantly improve the manuscript. Publisher Copyright: © 2021 Elsevier B.V.

PY - 2021/7/20

Y1 - 2021/7/20

N2 - As application of multiple metal isotopes can effectively constrain geochemical behavior of contaminants and assess contamination sources and pathways, field-scale studies on the geochemically interlinked fractionation of Zn and Cd isotopes in groundwater are needed. In this study, we collected groundwater samples from multi-level samplers downstream of tailings dumps as well as surface water, ore mineral, precipitate, and tailings samples at the Sambo and Buddeun metallic ore mines in South Korea, and analyzed their Zn, Cd, Pb, and sulfur isotopic compositions. Furthermore, isotopic ratios of ore mineral samples from additional four mines in South Korea (Dangdu, Dongbo, Gomyeong, Samgwang) were compared. A dual isotopic approach using Zn and Cd isotopes was used to assess fractionation processes, and Pb isotopic signatures reflecting their sources were assessed. Increasing trends of δ66Zn and δ114Cd with decreasing Zn and Cd concentrations were observed in groundwater, which was saturated with respect to ZnS (amorphous and sphalerite) and CdS (greenockite). Moreover, for some groundwater samples, δ66Zn showed a positive relationship with δ34SSO4. These results suggest that Zn and Cd are precipitated as sulfide following sulfate reduction. In the plot of δ66Zn against δ114Cd, relatively high and/or increasing δ66Zn in groundwater suggested the effect of fractionation due to sulfide precipitation, while variable and high δ114Cd values suggested the fractionation by adsorption and/or sulfide precipitation, which were based on positive fractionation factors for δ66Zn and δ114Cd during sulfide precipitation and mostly negative and positive fractionation factors for δ66Zn and δ114Cd, respectively, during adsorption. This study shows that the combined use of Zn and Cd isotopes in groundwater can effectively differentiate between adsorption and sulfide precipitation following sulfate reduction in groundwater. Additionally, the 208Pb/206Pb ratios of most water samples reflected those of ore and tailings samples, which verified usefulness of Pb isotopes in water in investigating Pb contamination sources.

AB - As application of multiple metal isotopes can effectively constrain geochemical behavior of contaminants and assess contamination sources and pathways, field-scale studies on the geochemically interlinked fractionation of Zn and Cd isotopes in groundwater are needed. In this study, we collected groundwater samples from multi-level samplers downstream of tailings dumps as well as surface water, ore mineral, precipitate, and tailings samples at the Sambo and Buddeun metallic ore mines in South Korea, and analyzed their Zn, Cd, Pb, and sulfur isotopic compositions. Furthermore, isotopic ratios of ore mineral samples from additional four mines in South Korea (Dangdu, Dongbo, Gomyeong, Samgwang) were compared. A dual isotopic approach using Zn and Cd isotopes was used to assess fractionation processes, and Pb isotopic signatures reflecting their sources were assessed. Increasing trends of δ66Zn and δ114Cd with decreasing Zn and Cd concentrations were observed in groundwater, which was saturated with respect to ZnS (amorphous and sphalerite) and CdS (greenockite). Moreover, for some groundwater samples, δ66Zn showed a positive relationship with δ34SSO4. These results suggest that Zn and Cd are precipitated as sulfide following sulfate reduction. In the plot of δ66Zn against δ114Cd, relatively high and/or increasing δ66Zn in groundwater suggested the effect of fractionation due to sulfide precipitation, while variable and high δ114Cd values suggested the fractionation by adsorption and/or sulfide precipitation, which were based on positive fractionation factors for δ66Zn and δ114Cd during sulfide precipitation and mostly negative and positive fractionation factors for δ66Zn and δ114Cd, respectively, during adsorption. This study shows that the combined use of Zn and Cd isotopes in groundwater can effectively differentiate between adsorption and sulfide precipitation following sulfate reduction in groundwater. Additionally, the 208Pb/206Pb ratios of most water samples reflected those of ore and tailings samples, which verified usefulness of Pb isotopes in water in investigating Pb contamination sources.

KW - Adsorption

KW - Fractionation

KW - Mining area

KW - Sulfide precipitation

KW - Zn and Cd isotopes

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U2 - 10.1016/j.scitotenv.2021.146453

DO - 10.1016/j.scitotenv.2021.146453

M3 - Article

C2 - 34030246

AN - SCOPUS:85102872728

SN - 0048-9697

VL - 779

JO - Science of the Total Environment

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M1 - 146453

ER -

Spatial patterns of Zn, Cd, and Pb isotopic compositions of ground and surface water in mine areas of South Korea reflecting isotopic fractionation during metal attenuation

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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