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Title: Origin of tungsten and geochemical controls on its occurrence and mobilization in shallow sediments from Fallon, Nevada, USA

Abstract

In this study, tungsten (W) occurrence and speciation was investigated in sediments collected from Fallon, Nevada where previous studies have linked elevated W levels in human body fluids to an unusual cluster of childhood leukemia cases. The speciation of sedimentary W was determined by μ-XRF mapping and μ-XANES. The W content of the analyzed surface sediments ranged between 81 and 25,908 mg/kg, which is significantly higher than the W content in deeper sediments which ranged from 37 to 373 mg/kg at 30 cm depth. The μ-XANES findings reveal that approximately 20–50% of the total W in the shallow sediment occurs in the metallic form (W0); the rest occurs in the oxide form (WVIO3). Because W0 does not occur naturally, its elevated concentrations in surface sediments point toward a possible local anthropogenic origin. The oxidation of metallic W0 with meteoric waters likely leads to the formation of WVIO3. The chief water-soluble W species was identified as WO42– by chromatographic separation and speciation modeling. These results led us to postulate that W0 particles from a currently unknown but local source(s) is (are) deposited onto the soils and/or surface sediments. The W0 in interaction with meteoric water is oxidized to WVIO3, and asmore » these sediment-water interactions progress, WO42– is formed in the water at pH ~7. Under pH < 7, and sufficient W concentrations, tungstate tends to polymerize, and polymerized species are less likely to adsorb onto sediments. Polymerized species have lower affinity than monomers, which leads to enhanced mobility of W.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8];  [1];  [2]
  1. Kansas State Univ., Manhattan, KS (United States)
  2. Kansas State Univ., Manhattan, KS (United States); Univ. of Texas at San Antonio, TX (United States)
  3. Univ. of Massachusetts, Boston, MA (United States)
  4. US Army Engineer Research and Development Center Vicksburg, MS (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Directorate
  6. Tulane Univ., New Orleans, LA (United States)
  7. Univ. of Arizona, Tucson, AZ (United States)
  8. Odyssey Research Institute, Tucson, AZ (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); United States-India Educational Foundation (USIEF)
OSTI Identifier:
1823625
Report Number(s):
BNL-222107-2021-JAAM
Journal ID: ISSN 0045-6535
Grant/Contract Number:  
SC0012704; EAR-1014971; EAR-1014946; 2203/FNPDR/2016
Resource Type:
Accepted Manuscript
Journal Name:
Chemosphere
Additional Journal Information:
Journal Volume: 260; Journal ID: ISSN 0045-6535
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; tungsten; sediment-water interface; childhood leukemia; μ-XRF mapping; water extractable tungsten

Citation Formats

Hobson, Chad, Kulkarni, Harshad V., Johannesson, Karen H., Bednar, Anthony, Tappero, Ryan, Mohajerin, T. Jade, Sheppard, Paul R., Witten, Mark L., Hettiarachchi, Ganga M., and Datta, Saugata. Origin of tungsten and geochemical controls on its occurrence and mobilization in shallow sediments from Fallon, Nevada, USA. United States: N. p., 2020. Web. doi:10.1016/j.chemosphere.2020.127577.
Hobson, Chad, Kulkarni, Harshad V., Johannesson, Karen H., Bednar, Anthony, Tappero, Ryan, Mohajerin, T. Jade, Sheppard, Paul R., Witten, Mark L., Hettiarachchi, Ganga M., & Datta, Saugata. Origin of tungsten and geochemical controls on its occurrence and mobilization in shallow sediments from Fallon, Nevada, USA. United States. https://doi.org/10.1016/j.chemosphere.2020.127577
Hobson, Chad, Kulkarni, Harshad V., Johannesson, Karen H., Bednar, Anthony, Tappero, Ryan, Mohajerin, T. Jade, Sheppard, Paul R., Witten, Mark L., Hettiarachchi, Ganga M., and Datta, Saugata. Sat . "Origin of tungsten and geochemical controls on its occurrence and mobilization in shallow sediments from Fallon, Nevada, USA". United States. https://doi.org/10.1016/j.chemosphere.2020.127577. https://www.osti.gov/servlets/purl/1823625.
@article{osti_1823625,
title = {Origin of tungsten and geochemical controls on its occurrence and mobilization in shallow sediments from Fallon, Nevada, USA},
author = {Hobson, Chad and Kulkarni, Harshad V. and Johannesson, Karen H. and Bednar, Anthony and Tappero, Ryan and Mohajerin, T. Jade and Sheppard, Paul R. and Witten, Mark L. and Hettiarachchi, Ganga M. and Datta, Saugata},
abstractNote = {In this study, tungsten (W) occurrence and speciation was investigated in sediments collected from Fallon, Nevada where previous studies have linked elevated W levels in human body fluids to an unusual cluster of childhood leukemia cases. The speciation of sedimentary W was determined by μ-XRF mapping and μ-XANES. The W content of the analyzed surface sediments ranged between 81 and 25,908 mg/kg, which is significantly higher than the W content in deeper sediments which ranged from 37 to 373 mg/kg at 30 cm depth. The μ-XANES findings reveal that approximately 20–50% of the total W in the shallow sediment occurs in the metallic form (W0); the rest occurs in the oxide form (WVIO3). Because W0 does not occur naturally, its elevated concentrations in surface sediments point toward a possible local anthropogenic origin. The oxidation of metallic W0 with meteoric waters likely leads to the formation of WVIO3. The chief water-soluble W species was identified as WO42– by chromatographic separation and speciation modeling. These results led us to postulate that W0 particles from a currently unknown but local source(s) is (are) deposited onto the soils and/or surface sediments. The W0 in interaction with meteoric water is oxidized to WVIO3, and as these sediment-water interactions progress, WO42– is formed in the water at pH ~7. Under pH < 7, and sufficient W concentrations, tungstate tends to polymerize, and polymerized species are less likely to adsorb onto sediments. Polymerized species have lower affinity than monomers, which leads to enhanced mobility of W.},
doi = {10.1016/j.chemosphere.2020.127577},
journal = {Chemosphere},
number = ,
volume = 260,
place = {United States},
year = {Sat Jul 11 00:00:00 EDT 2020},
month = {Sat Jul 11 00:00:00 EDT 2020}
}

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