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Carbonate-Enhanced Transformation of Ferrihydrite to Hematite

  • Ying Li
    Ying Li
    Department of Natural Resources and Environmental Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
    More by Ying Li
  • Meijun Yang
    Meijun Yang
    CAS Key Laboratory of Mineralogy and Metallogeny/Guangdong Provincial Key Laboratory of Mineral Physics and Materials, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China
    University of Chinese Academy of Sciences, Beijing 100049, PR China
    More by Meijun Yang
  • Martin Pentrak
    Martin Pentrak
    Illinois State Geological Survey, Prairie Research Institute, University of Illinois at Urbana-Champaign, Champaign, Illinois 61820, United States
  • Hongping He
    Hongping He
    CAS Key Laboratory of Mineralogy and Metallogeny/Guangdong Provincial Key Laboratory of Mineral Physics and Materials, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China
    University of Chinese Academy of Sciences, Beijing 100049, PR China
    More by Hongping He
  • , and 
  • Yuji Arai*
    Yuji Arai
    Department of Natural Resources and Environmental Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
    *E-mail: [email protected]
    More by Yuji Arai
Cite this: Environ. Sci. Technol. 2020, 54, 21, 13701–13708
Publication Date (Web):October 22, 2020
https://doi.org/10.1021/acs.est.0c04043
Copyright © 2020 American Chemical Society

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    Abstract

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    An elevated activity of (bi)carbonate in soils and sediments (pCO2, ∼2%) above current atmospheric CO2 (∼0.04%) could influence the iron cycling in mineral-water interfacial chemistry. However, the impact of (bi)carbonate on mineral transformation is unclear. Here, a model short range-ordered iron oxyhydroxide, two-line ferrihydrite, was used to evaluate the impact of (bi)carbonate on mineral transformation at near-neutral pH using experimental geochemistry, X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, and Fourier transform infrared spectroscopy. Results showed that (bi)carbonate promoted the transformation of ferrihydrite to hematite and retarded the goethite formation. As pCO2 increased from 408 to 20,000 ppmv at 40 °C, the transformation efficiency of ferrihydrite increased from 53 to 95%, and the formation of hematite increased from 13 to 76%. During the formation of hematite, a terminal ligand on a Fe(III)O6 octahedral monomer such as a hydroxyl or water was displaced to form Fe(III)O6 octahedral dimers and/or polymers. Because the Fe–O bond of ≡(Fe–O)2–CO is much weaker than that of ≡Fe–O–H, the −O2CO group can be more easily replaced by two terminal −OH groups; the dehydration/rearrangement between Fe(III)O6 octahedral monomers was enhanced under high pCO2. Results suggest that high carbonate activity is an important geochemical parameter controlling the occurrence of hematite in oxic environments and, in turn, iron cycling in the critical zone.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c04043.

    • Results of LCF of Fe K-edge EXAFS spectra and peak deconvolution of FTIR spectra, EXAFS spectra and fits, effect of carbonate on goethite and hematite formation, pH variations in unbuffered systems, effect of ionic strength on ferrihydrite transformation, and schematic diagram of shared charge in different ions (PDF)

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