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Title: X-ray fluorescence mapping of mercury on suspended mineral particles and diatoms in a contaminated freshwater system

Abstract

Mercury (Hg) bioavailability and geochemical cycling is affected by its partitioning between the aqueous and particulate phases. We applied a synchrotron-based X-ray fluorescence (XRF) microprobe to visualize and quantify directly the spatial localization of Hg and its correlations with other elements of interest on suspended particles from a Hg-contaminated freshwater system. Up to 175 μg g−1 Hg is found on suspended particles, but less than 0.01% is in the form of methylmercury. Mercury is heterogeneously distributed among phytoplankton (e.g., diatoms) and mineral particles that are rich in iron oxides and natural organic matter (NOM). The diatom-bound Hg is mostly found on outer surfaces of the cells, suggesting passive sorption of Hg on diatoms. Our results indicate that localized sorption of Hg onto suspended particles, including diatoms and NOM-coated oxide minerals, may play an important role in affecting the partitioning, reactivity, and biogeochemical cycling of Hg in natural aquatic environments.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1198214
Alternate Identifier(s):
OSTI ID: 1132978
Grant/Contract Number:  
AC02-06CH11357; AC05-00OR22725
Resource Type:
Published Article
Journal Name:
Biogeosciences (Online)
Additional Journal Information:
Journal Name: Biogeosciences (Online) Journal Volume: 11 Journal Issue: 18; Journal ID: ISSN 1726-4189
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Mercury; Diatom; mineral; particulates; X-ray

Citation Formats

Gu, B., Mishra, B., Miller, C., Wang, W., Lai, B., Brooks, S. C., Kemner, K. M., and Liang, L. X-ray fluorescence mapping of mercury on suspended mineral particles and diatoms in a contaminated freshwater system. Germany: N. p., 2014. Web. doi:10.5194/bg-11-5259-2014.
Gu, B., Mishra, B., Miller, C., Wang, W., Lai, B., Brooks, S. C., Kemner, K. M., & Liang, L. X-ray fluorescence mapping of mercury on suspended mineral particles and diatoms in a contaminated freshwater system. Germany. https://doi.org/10.5194/bg-11-5259-2014
Gu, B., Mishra, B., Miller, C., Wang, W., Lai, B., Brooks, S. C., Kemner, K. M., and Liang, L. Tue . "X-ray fluorescence mapping of mercury on suspended mineral particles and diatoms in a contaminated freshwater system". Germany. https://doi.org/10.5194/bg-11-5259-2014.
@article{osti_1198214,
title = {X-ray fluorescence mapping of mercury on suspended mineral particles and diatoms in a contaminated freshwater system},
author = {Gu, B. and Mishra, B. and Miller, C. and Wang, W. and Lai, B. and Brooks, S. C. and Kemner, K. M. and Liang, L.},
abstractNote = {Mercury (Hg) bioavailability and geochemical cycling is affected by its partitioning between the aqueous and particulate phases. We applied a synchrotron-based X-ray fluorescence (XRF) microprobe to visualize and quantify directly the spatial localization of Hg and its correlations with other elements of interest on suspended particles from a Hg-contaminated freshwater system. Up to 175 μg g−1 Hg is found on suspended particles, but less than 0.01% is in the form of methylmercury. Mercury is heterogeneously distributed among phytoplankton (e.g., diatoms) and mineral particles that are rich in iron oxides and natural organic matter (NOM). The diatom-bound Hg is mostly found on outer surfaces of the cells, suggesting passive sorption of Hg on diatoms. Our results indicate that localized sorption of Hg onto suspended particles, including diatoms and NOM-coated oxide minerals, may play an important role in affecting the partitioning, reactivity, and biogeochemical cycling of Hg in natural aquatic environments.},
doi = {10.5194/bg-11-5259-2014},
journal = {Biogeosciences (Online)},
number = 18,
volume = 11,
place = {Germany},
year = {Tue Sep 30 00:00:00 EDT 2014},
month = {Tue Sep 30 00:00:00 EDT 2014}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.5194/bg-11-5259-2014

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Cited by: 27 works
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Works referenced in this record:

Determination of mercury in polluted soils surrounding a chlor-alkali plant
journal, April 2006


Kinetic Controls on the Complexation between Mercury and Dissolved Organic Matter in a Contaminated Environment
journal, November 2009

  • Miller, Carrie L.; Southworth, George; Brooks, Scott
  • Environmental Science & Technology, Vol. 43, Issue 22
  • DOI: 10.1021/es901891t

The Influence of Aluminum on Iron Oxides. XV. Al-for-Fe Substitution in Synthetic Lepidocrocite
journal, January 1990


Mixed-Valence Cytoplasmic Iron Granules Are Linked to Anaerobic Respiration
journal, December 2006

  • Glasauer, S.; Langley, S.; Boyanov, M.
  • Applied and Environmental Microbiology, Vol. 73, Issue 3
  • DOI: 10.1128/AEM.01492-06

Mercury distribution in relation to iron and manganese in the waters of the St. Lawrence river
journal, June 1998


Bioaccumulation of Mercury and Methylmercury
book, January 1995


A Structural Model for Natural Siliceous Ferrihydrite
journal, January 1992


Metallothionein-Like Multinuclear Clusters of Mercury(II) and Sulfur in Peat
journal, September 2011

  • Nagy, Kathryn L.; Manceau, Alain; Gasper, Jarrod D.
  • Environmental Science & Technology, Vol. 45, Issue 17
  • DOI: 10.1021/es201025v

Microchemical Element Imaging of Yeast and Human Cells Using Synchrotron X-ray Microprobe with Kirkpatrick−Baez Optics
journal, January 2004

  • Ortega, Richard; Bohic, Sylvain; Tucoulou, Rémi
  • Analytical Chemistry, Vol. 76, Issue 2
  • DOI: 10.1021/ac035037r

Characteristics of mercury speciation in Minnesota rivers and streams
journal, July 2008


Quantitative 3D elemental microtomography of Cyclotella meneghiniana at 400-nm resolution
journal, August 2010

  • de Jonge, M. D.; Holzner, C.; Baines, S. B.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 36
  • DOI: 10.1073/pnas.1001469107

Adsorption and desorption of different organic matter fractions on iron oxide
journal, January 1995


Binding Constants of Mercury and Dissolved Organic Matter Determined by a Modified Ion Exchange Technique
journal, April 2011

  • Dong, Wenming; Bian, Yongrong; Liang, Liyuan
  • Environmental Science & Technology, Vol. 45, Issue 8
  • DOI: 10.1021/es104207g

Solving mercury (Hg) speciation in soil samples by synchrotron X-ray microspectroscopic techniques
journal, August 2010


Patterns of Mercury Accumulation among Seston in Lakes of the Adirondack Mountains, New York
journal, July 2009

  • Adams, Ryan M.; Twiss, Michael R.; Driscoll, Charles T.
  • Environmental Science & Technology, Vol. 43, Issue 13
  • DOI: 10.1021/es900409b

Elemental and Redox Analysis of Single Bacterial Cells by X-ray Microbeam Analysis
journal, October 2004


Mercury and methylmercury, in individual zooplankton: Implications for bioaccumulation
journal, September 1992


Uptake, Toxicity, and Trophic Transfer of Mercury in a Coastal Diatom
journal, January 1996

  • Mason, Robert P.; Reinfelder, John R.; Morel, François M. M.
  • Environmental Science & Technology, Vol. 30, Issue 6
  • DOI: 10.1021/es950373d

Contribution of suspended particulate matter and zooplankton to MeHg contamination of the food chain in midnorthern Quebec (Canada) reservoirs
journal, April 1997

  • Plourde, Y.; Lucotte, M.; Pichet, P.
  • Canadian Journal of Fisheries and Aquatic Sciences, Vol. 54, Issue 4
  • DOI: 10.1139/f96-340

Effect of carboxylic and thiol ligands (oxalate, cysteine) on the kinetics of desorption of Hg(II) from kaolinite
journal, June 2010

  • U. Senevirathna, Wasana; Zhang, Hong; Gu, Baohua
  • Water, Air, & Soil Pollution, Vol. 215, Issue 1-4
  • DOI: 10.1007/s11270-010-0500-3

Adsorption on Hydrous Oxides. iii. Fulvic acid and Humic acid on Goethite, Gibbsite and Imogolite
journal, June 1977


A hard x-ray scanning microprobe for fluorescence imaging and microdiffraction at the advanced photon source
conference, January 2000

  • Cai, Z.
  • Sixth international conference on x-ray microscopy (XRM99), AIP Conference Proceedings
  • DOI: 10.1063/1.1291193

Mercury Reduction and Oxidation by Reduced Natural Organic Matter in Anoxic Environments
journal, November 2011

  • Zheng, Wang; Liang, Liyuan; Gu, Baohua
  • Environmental Science & Technology, Vol. 46, Issue 1
  • DOI: 10.1021/es203402p

Oxidation and methylation of dissolved elemental mercury by anaerobic bacteria
journal, August 2013

  • Hu, Haiyan; Lin, Hui; Zheng, Wang
  • Nature Geoscience, Vol. 6, Issue 9
  • DOI: 10.1038/ngeo1894

Formation of Mercuric Sulfide in Soil
journal, November 1997

  • Barnett, Mark O.; Harris, Lawerence A.; Turner, Ralph R.
  • Environmental Science & Technology, Vol. 31, Issue 11
  • DOI: 10.1021/es960389j

Complexation of Mercury(II) in Soil Organic Matter:  EXAFS Evidence for Linear Two-Coordination with Reduced Sulfur Groups
journal, July 2006

  • Skyllberg, Ulf; Bloom, Paul R.; Qian, Jin
  • Environmental Science & Technology, Vol. 40, Issue 13
  • DOI: 10.1021/es0600577

Cadmium and lead interaction with diatom surfaces: A combined thermodynamic and kinetic approach
journal, August 2007

  • Gélabert, A.; Pokrovsky, O. S.; Schott, J.
  • Geochimica et Cosmochimica Acta, Vol. 71, Issue 15
  • DOI: 10.1016/j.gca.2007.04.034

Quantifying Trace Elements in Individual Aquatic Protist Cells with a Synchrotron X-ray Fluorescence Microprobe
journal, August 2003

  • Twining, Benjamin S.; Baines, Stephen B.; Fisher, Nicholas S.
  • Analytical Chemistry, Vol. 75, Issue 15
  • DOI: 10.1021/ac034227z

Arsenic Sequestration by Ferric Iron Plaque on Cattail Roots
journal, November 2004

  • Blute, Nicole Keon; Brabander, Daniel J.; Hemond, Harold F.
  • Environmental Science & Technology, Vol. 38, Issue 22
  • DOI: 10.1021/es049448g

The protonation of phosphate on the surface of goethite as studied by CIR-FTIR and electrophoretic mobility
journal, March 1990

  • Tejedor-Tejedor, M. Isabel; Anderson, Marc A.
  • Langmuir, Vol. 6, Issue 3
  • DOI: 10.1021/la00093a015

Distribution of particulate, colloidal, and dissolved mercury in San Francisco Bay estuary. 1. Total mercury
journal, July 2003


The Genetic Basis for Bacterial Mercury Methylation
journal, February 2013


Adsorption and desorption of natural organic matter on iron oxide: mechanisms and models
journal, January 1994

  • Gu, Baohua.; Schmitt, Juergen.; Chen, Zhihong.
  • Environmental Science & Technology, Vol. 28, Issue 1
  • DOI: 10.1021/es00050a007

Mercury Reduction and Cell-Surface Adsorption by Geobacter sulfurreducens PCA
journal, September 2013

  • Hu, Haiyan; Lin, Hui; Zheng, Wang
  • Environmental Science & Technology, Vol. 47, Issue 19
  • DOI: 10.1021/es400527m

Roles of dissolved organic matter in the speciation of mercury and methylmercury in a contaminated ecosystem in Oak Ridge, Tennessee
journal, January 2010

  • Dong, Wenming; Liang, Liyuan; Brooks, Scott
  • Environmental Chemistry, Vol. 7, Issue 1
  • DOI: 10.1071/EN09091

Accumulation of Inorganic and Methylmercury by Freshwater Phytoplankton in Two Contrasting Water Bodies
journal, January 2007

  • Pickhardt, Paul C.; Fisher, Nicholas S.
  • Environmental Science & Technology, Vol. 41, Issue 1
  • DOI: 10.1021/es060966w

History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant
journal, January 2011


Mercury reduction and complexation by natural organic matter in anoxic environments
journal, January 2011

  • Gu, B.; Bian, Y.; Miller, C. L.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 4
  • DOI: 10.1073/pnas.1008747108