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Title: Macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite with the effects of dissolved carbonates under anoxic conditions

Abstract

Manganese and its compounds have been extensively researched because of their far-reaching roles in a wide range of biogeochemical processes in natural systems. The (ad)sorption behavior of Mn(II), however, is poorly understood despite its important role as the primary reaction step for surface-catalyzed Mn(II) oxidation that is the principal abiotic process forming various Mn (oxyhydr)oxides in nature. Here, we systematically examined Mn(II) (ad)sorption to one of the most common natural sorbents, goethite, in oxygen- and carbonate-free systems. Traditional sorption edge and isotherm experiments were conducted by varying sorbate-to-sorbent ratio (0.027–15 μmol∙m-2) and solution pH (pH 5.0–9.0). The effects of dissolved carbonates on Mn(II) sorption were also assessed in a range of naturally prevalent concentrations (0.5–10 mM NaHCO3). The Mn(II) uptake on goethite followed a typical Langmuir isotherm in the absence of dissolved carbonates, with increasing maximum adsorption capacities (Γmax) from 0.19 at pH 6.5 to 3.4 μmol∙m-2 at pH 9.0. The presence of dissolved carbonates raised the extent of Mn(II) adsorption, which appeared to be directly correspondent to that of the adsorption of dissolved carbonates. Extended X-ray absorption fine structure (EXAFS) analysis indicated that Mn(II) predominantly formed inner-sphere binuclear bidentate surface complexes. Mn(II) uptake became deviated from the Langmuir modelmore » and showed a clear indication of surface precipitation when the Mn(II) sorption density (Γ) exceeded a threshold value in a given solution composition. This secondary Mn(II) phase was identified as rhodochrosite using X-ray diffraction (XRD) and transmission electron microscope (TEM). Furthermore, it would be plausible that a minor fraction of adsorbed Mn(II) coexisted with the secondary rhodochrosite according to a linear combination fitting (LCF) of the X-ray absorption near edge structure (XANES) spectra of Mn reference and samples. These systematic investigations of the macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite provide a critical avenue for disentangling surface-catalytic Mn(II) oxidation processes, which ultimately lead to the formation of diverse Mn (oxyhydr)oxides in the environment.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [3];  [4]
+ Show Author Affiliations
  1. Yonsei Univ., Seoul (Korea, Republic of)
  2. Kyushu Univ., Fukuoka (Japan)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Yonsei Univ., Seoul (Korea, Republic of); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Research Foundation of Korea (NRF); Japan Society for the Promotion of Science (JSPS) - KAKENHI; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1617647
Alternate Identifier(s):
OSTI ID: 1615557
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 277; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; manganese; goethite; oxidation; heterogeneous catalysis; sorption isotherm

Citation Formats

Namgung, Seonyi, Guo, Binglin, Sasaki, Keiko, Lee, Sang Soo, and Lee, Giehyeon. Macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite with the effects of dissolved carbonates under anoxic conditions. United States: N. p., 2020. Web. doi:10.1016/j.gca.2020.03.036.
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Namgung, Seonyi, Guo, Binglin, Sasaki, Keiko, Lee, Sang Soo, & Lee, Giehyeon. Macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite with the effects of dissolved carbonates under anoxic conditions. United States. https://doi.org/10.1016/j.gca.2020.03.036
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Namgung, Seonyi, Guo, Binglin, Sasaki, Keiko, Lee, Sang Soo, and Lee, Giehyeon. Sat . "Macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite with the effects of dissolved carbonates under anoxic conditions". United States. https://doi.org/10.1016/j.gca.2020.03.036. https://www.osti.gov/servlets/purl/1617647.
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@article{osti_1617647,
title = {Macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite with the effects of dissolved carbonates under anoxic conditions},
author = {Namgung, Seonyi and Guo, Binglin and Sasaki, Keiko and Lee, Sang Soo and Lee, Giehyeon},
abstractNote = {Manganese and its compounds have been extensively researched because of their far-reaching roles in a wide range of biogeochemical processes in natural systems. The (ad)sorption behavior of Mn(II), however, is poorly understood despite its important role as the primary reaction step for surface-catalyzed Mn(II) oxidation that is the principal abiotic process forming various Mn (oxyhydr)oxides in nature. Here, we systematically examined Mn(II) (ad)sorption to one of the most common natural sorbents, goethite, in oxygen- and carbonate-free systems. Traditional sorption edge and isotherm experiments were conducted by varying sorbate-to-sorbent ratio (0.027–15 μmol∙m-2) and solution pH (pH 5.0–9.0). The effects of dissolved carbonates on Mn(II) sorption were also assessed in a range of naturally prevalent concentrations (0.5–10 mM NaHCO3). The Mn(II) uptake on goethite followed a typical Langmuir isotherm in the absence of dissolved carbonates, with increasing maximum adsorption capacities (Γmax) from 0.19 at pH 6.5 to 3.4 μmol∙m-2 at pH 9.0. The presence of dissolved carbonates raised the extent of Mn(II) adsorption, which appeared to be directly correspondent to that of the adsorption of dissolved carbonates. Extended X-ray absorption fine structure (EXAFS) analysis indicated that Mn(II) predominantly formed inner-sphere binuclear bidentate surface complexes. Mn(II) uptake became deviated from the Langmuir model and showed a clear indication of surface precipitation when the Mn(II) sorption density (Γ) exceeded a threshold value in a given solution composition. This secondary Mn(II) phase was identified as rhodochrosite using X-ray diffraction (XRD) and transmission electron microscope (TEM). Furthermore, it would be plausible that a minor fraction of adsorbed Mn(II) coexisted with the secondary rhodochrosite according to a linear combination fitting (LCF) of the X-ray absorption near edge structure (XANES) spectra of Mn reference and samples. These systematic investigations of the macroscopic and microscopic behaviors of Mn(II) (ad)sorption to goethite provide a critical avenue for disentangling surface-catalytic Mn(II) oxidation processes, which ultimately lead to the formation of diverse Mn (oxyhydr)oxides in the environment.},
doi = {10.1016/j.gca.2020.03.036},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 277,
place = {United States},
year = {Sat Apr 04 00:00:00 EDT 2020},
month = {Sat Apr 04 00:00:00 EDT 2020}
}
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Reactions at Oxide Surfaces. 1. Oxidation of As(III) by Synthetic Birnessite
journal, August 1995

  • Scott, Michael J.; Morgan, James J.
  • Environmental Science & Technology, Vol. 29, Issue 8
  • DOI: 10.1021/es00008a006

Structure and Stability of Cd2+ Surface Complexes on Ferric Oxides
journal, November 1994

  • Spadini, Lorenzo; Manceau, Alain; Schindler, Paul W.
  • Journal of Colloid and Interface Science, Vol. 168, Issue 1
  • DOI: 10.1006/jcis.1994.1395

Kinetics of rhodochrosite crystal growth at 25°C: The role of surface speciation
journal, February 1997

In Situ Infrared Speciation of Adsorbed Carbonate on Aluminum and Iron Oxides
journal, January 1997

Effects of oxygen and redox oscillation on degradation of cell-associated lipids in surficial marine sediments
journal, June 2002

Formation of Cd precipitates on γ-Al2O3: Implications for Cd sequestration in the environment
journal, May 2019

Oxidative removal of Mn(II) from solution catalysed by the γ-FeOOH (lepidocrocite) surface
journal, December 1981

Goethite adsorption of Cu(II), Pb(II), Cd(II), and Zn(II) in the presence of sulfate: Properties of the ternary complex
journal, March 2009

  • Swedlund, Peter J.; Webster, Jenny G.; Miskelly, Gordon M.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 6
  • DOI: 10.1016/j.gca.2008.12.007

Evidence for a Dynamic Cycle between Mn and Co in the Water Column of a Stratified Lake
journal, February 2002

  • Taillefert, Martial; MacGregor, Barbara J.; Gaillard, Jean-François
  • Environmental Science & Technology, Vol. 36, Issue 3
  • DOI: 10.1021/es010915t

X-ray Absorption Near Edge Structure Study of Lead Sorption on Phosphate-Treated Kaolinite
journal, February 2009

  • Taylor, Robert W.; Bleam, William F.; Ranatunga, Thilini D.
  • Environmental Science & Technology, Vol. 43, Issue 3
  • DOI: 10.1021/es8020183

Manganese(II) oxidation in the suboxic zone of the Black Sea
journal, January 1991

BIOGENIC MANGANESE OXIDES: Properties and Mechanisms of Formation
journal, May 2004

Geomicrobiology of manganese(II) oxidation
journal, September 2005

  • Tebo, Bradley M.; Johnson, Hope A.; McCarthy, James K.
  • Trends in Microbiology, Vol. 13, Issue 9
  • DOI: 10.1016/j.tim.2005.07.009

Manganese, iron and sulfur cycling in a coastal marine sediment, Aarhus bay, Denmark
journal, December 1994

Adsorption and Precipitation of Aqueous Zn(II) on Alumina Powders
journal, November 2000

  • Trainor, Thomas P.; Brown, Gordon E.; Parks, George A.
  • Journal of Colloid and Interface Science, Vol. 231, Issue 2
  • DOI: 10.1006/jcis.2000.7111

Adsorption of metal ions onto goethite: single-adsorbate and competitive systems
journal, October 2001

  • Trivedi, Paras; Axe, Lisa; Dyer, James
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 191, Issue 1-2
  • DOI: 10.1016/S0927-7757(01)00768-3

Surface Precipitation of Co(II)(aq) on Al2O3
journal, March 1997

  • Towle, Steven N.; Bargar, John R.; Brown, Gordon E.
  • Journal of Colloid and Interface Science, Vol. 187, Issue 1
  • DOI: 10.1006/jcis.1996.4539

Adsorption of Cu(II), Cd(II), Zn(II), Mn(II) and Fe(III) ions by tannic acid immobilised activated carbon
journal, January 2006

Complexation of carbonate species at the goethite surface: Implications for adsorption of metal ions in natural waters
journal, May 1994

  • van Geen, Alexander; Robertson, Alexander P.; Leckie, James O.
  • Geochimica et Cosmochimica Acta, Vol. 58, Issue 9
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Biological oxidation of manganese in soils
journal, December 1973

Multisite Adsorption of Cadmium on Goethite
journal, November 1996

  • Venema, Peter; Hiemstra, Tjisse; van Riemsdijk, Willem H.
  • Journal of Colloid and Interface Science, Vol. 183, Issue 2
  • DOI: 10.1006/jcis.1996.0575

Carbonate adsorption on goethite under closed and open CO2 conditions
journal, November 2000

Surface Complexation Modeling of Carbonate Effects on the Adsorption of Cr(VI), Pb(II), and U(VI) on Goethite
journal, October 2001

  • Villalobos, Mario; Trotz, Maya A.; Leckie, James O.
  • Environmental Science & Technology, Vol. 35, Issue 19
  • DOI: 10.1021/es001748k

Characterization of the manganese oxide produced by pseudomonas putida strain MnB1
journal, July 2003

Variability in goethite surface site density: evidence from proton and carbonate sorption
journal, December 2003

  • Villalobos, Mario; Trotz, Maya A.; Leckie, James O.
  • Journal of Colloid and Interface Science, Vol. 268, Issue 2
  • DOI: 10.1016/j.jcis.2003.07.044

Mechanisms of Pb(II) Sorption on a Biogenic Manganese Oxide
journal, January 2005

  • Villalobos, Mario; Bargar, John; Sposito, Garrison
  • Environmental Science & Technology, Vol. 39, Issue 2
  • DOI: 10.1021/es049434a

From adsorption to precipitation: Sorption of Mn2+ on FeCO3(s)
journal, November 1989

Surface and complexation effects on the rate of Mn(II) oxidation in natural waters
journal, September 1980

Oxidative removal of aqueous steroid estrogens by manganese oxides
journal, December 2008

Removal of copper, nickel, cobalt and manganese from aqueous solution by kaolinite
journal, February 2003

Competitive Microbially and Mn Oxide Mediated Redox Processes Controlling Arsenic Speciation and Partitioning
journal, July 2011

  • Ying, Samantha C.; Kocar, Benjamin D.; Griffis, Sarah D.
  • Environmental Science & Technology, Vol. 45, Issue 13
  • DOI: 10.1021/es200351m

Sorption of divalent metals on calcite
journal, June 1991

Oxidative Transformation of Triclosan and Chlorophene by Manganese Oxides
journal, June 2003

  • Zhang, Huichun; Huang, Ching-Hua
  • Environmental Science & Technology, Vol. 37, Issue 11
  • DOI: 10.1021/es026190q
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