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Microbially mediated iron redox cycling of subsurface sediments from Hanford Site, Washington State, USA

Journal Article · · Chemical Geology
 [1];  [2];  [3];  [4];  [5];  [5]
  1. Miami Univ., Oxford, OH (United States); OSTI
  2. Miami Univ., Oxford, OH (United States); China Univ. of Geosciences, Beijing (China)
  3. Miami Univ., Oxford, OH (United States)
  4. Miami Univ., Oxford, OH (United States); Univ. of Alaska, Anchorage, AK (United States)
  5. Univ. of Illinois at Urbana-Champaign, IL (United States)
Iron-bearing clay minerals are predominant in soils and sediments, and they undergo oxidation-reduction cycles as a result of natural processes such as wetting/drying cycles and plant root respiration. However, the kinetics and mechanisms of multiple redox cycles of iron in clay-rich sediments and consequences of such cycling on sediment properties are poorly understood. The objective of this study was to understand how multiple redox cycles of Fe in clay-rich sediment affect the rate and extent of Fe bioreduction and the physicochemical properties of the sediment. A natural sediment sample containing Fe-bearing montmorillonite from Hanford, Washington, USA was size-fractionated [2.0 to 0.5 μm (Hanford-C) and 0.5 to 0.02 μm (Hanford-F)] and redox-cycled for four times. Bioreduction was achieved utilizing Geobacter sulfurreducens and re-oxidization was performed with sparged air. Time-course change of total Fe (II) was monitored to measure the rate and extent of Fe (III) bioreduction. Redox-cycled sediments were characterized to determine the physicochemical changes. Both the initial rate and extent of bioreduction fluctuated across the four redox cycles, but they ultimately decreased from 5.3 μmol g-1 h-1 and 22.9% to nearly zero by the fourth cycle. These fluctuation patterns were likely due to a combined effect of reductive dissolution of small/poorly crystalline clay particles (by 3–5%) and clay mineral structural changes, as evidenced by redox induced changes of aqueous chemistry, surface area, cation exchange capacity, mineralogy, and Mössbauer parameters. Once these small/poorly crystalline clay particles were dissolved, structural Fe in residual larger and more crystalline clay particles was largely reversible across additional redox cycles, as revealed by Mössbauer spectroscopy through the first three cycles.
Research Organization:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0005333
OSTI ID:
1801669
Alternate ID(s):
OSTI ID: 1619376
Journal Information:
Chemical Geology, Journal Name: Chemical Geology Vol. 546; ISSN 0009-2541
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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