Long-term sequestration of nickel in mackinawite formed by Desulfovibrio capillatus upon Fe(III)-citrate reduction in the presence of thiosulfate

Ikogou, Maya; Ona-Nguéma, Georges; Juillot, Farid; Pape, Pierre Le; Menguy, Nicolas; Richeux, Nicolas; Guigner, Jean‐Michel; Noël, Vincent; Brest, Jessica; Baptiste, Benoı̂t; Morin, Guillaume

doi:10.1016/j.apgeochem.2017.02.019

Cited by 26 publications

(16 citation statements)

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“…The energy positions correspond to those expected for mackinawite‐like (FeS) (2470.9 eV) and pyrite‐like (FeS 2 ) (2472.3 eV). [ 50,51 ] Since FeS can serve as a precursor for pyrite formation in the presence of H 2 S, [ 39 ] it is likely that different S/Fe doses formed different amounts of H 2 S and FeS in the synthesis, and thus resulted in different amounts of FeS and FeS 2 . In addition, S K‐edge XANES spectra (Figure 2d) indicate the presence of “L‐cystine‐like” (R‐SS‐R') phases in the [S/Fe] measured = 0.01 sample, and some sulfate precipitation as FeSO 4(s) in all samples.…”

Section: Figurementioning

confidence: 99%

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

et al. 2020

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radionuclides. [12][13][14][15][16][17] However, NZVI is an indiscriminate reductant that also readily reduces water to form hydrogen gas (Fe 0 + 2H 2 O → Fe 2+ + 2OH − + H 2(g) ). [18] This unwanted side reaction consumes the reducing capacity of the NZVI, decreasing its reactive lifetime, and increases the amount and cost of NZVI required for remediation. Several approaches have been proposed to increase the reactivity or stability of NZVI during remediation, including encapsulating them with polymers or into silica matrices, [15,19] doping them with noble metals like Pd or Pt, [20,21] and supporting them onto carbon matrices like carbon nanotubes or graphene. [22,23] While these approaches improve the injectability of the materials into the subsurface, none have improved the selectivity of NZVI for contaminants over water while still maintaining high reactivity with the target groundwater contaminants. An ideal material for groundwater remediation should possess both high reactivity and selectivity, [24] where the contaminant outcompetes water for reactive sites.Recently, it was shown by us and others that the sulfidation of NZVI lowers its reactivity with water and other non-target hydrophilic contaminants (e.g., NO 3 − ), while increasing its reactivity with target contaminants like chlorinated solvents Sulfidized nanoscale zerovalent iron (SNZVI) is a promising material for groundwater remediation. However, the relationships between sulfur content and speciation and the properties of SNZVI materials are unknown, preventing rational design. Here, the effects of sulfur on the crystalline structure, hydrophobicity, sulfur speciation, corrosion potential, and electron transfer resistance are determined. Sulfur incorporation extended the nano-Fe 0 BCC lattice parameter, reduced the Fe local vacancies, and lowered the resistance to electron transfer. Impacts of the main sulfur species (FeS and FeS 2 ) on hydrophobicity (water contact angles) are consistent with density functional theory calculations for these FeS x phases. These properties well explain the reactivity and selectivity of SNZVI during the reductive dechlorination of trichloroethylene (TCE), a hydrophobic groundwater contaminant. Controlling the amount and speciation of sulfur in the SNZVI made it highly reactive (up to 0.41 L m −2 d −1 ) and selective for TCE degradation over water (up to 240 moles TCE per mole H 2 O), with an electron efficiency of up to 70%, and these values are 54-fold, 98-fold, and 160-fold higher than for NZVI, respectively. These findings can guide the rational design of robust SNZVI with properties tailored for specific application scenarios.Highly redox active materials are an important tool for the degradation of refractory organic water and soil contaminants. [1][2][3][4][5][6][7] Nanoscale zero valent (NZVI) has been used for in situ groundwater remediation for more than two decades. [8][9][10][11][12] NZVI is a strong reductant that readily dechlorinates chlorinated solvents and antibiotics, and reduces and immobilizes h...

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Section: Figurementioning

confidence: 99%

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

et al. 2020

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“…This reaction is kinetically fast (Rickard, 1995), explaining the presence of amorphous iron sulfide (or disordered mackinawite) as the first product of abiotic pyrite synthesis in both ferrous and ferric-sulfide systems (Schoonen and Barnes, 1991;Wei and Osseo-Asare, 1997). Similarly, laboratory sulfate-reducing bacteria pure cultures have mainly yielded the formation of amorphous FeS (Fortin et al, 1994;Williams et al, 2005;Ntarlagiannis et al, 2005;Peltier et al, 2011;Stanley and Southam, 2018) or of well-crystallized mackinawite (Rickard, 1969b;Ivarson and Hallberg, 1976;Zhou et al, 2014;Ikogou et al, 2017;Picard et al, 2018). Some of these studies also detected greigite in long-term experiments (Rickard, 1969b;Picard et al, 2018) with excess of electron donor (Zhou et al, 2014).…”

Section: First Stages Of Iron Sulfide Formation (1 Week)mentioning

confidence: 99%

“…However, due to the huge diversity of bacteria in these enrichments, especially iron-and sulfur-cycling bacteria (Lehours et al, 2009;Sitte et al, 2013;Zeng et al, 2018;Berg et al, 2019), deciphering the specific role of sulfate-reducing bacteria is tricky. Despite several attempts at iron sulfide biomineralization in pure sulfate-reducing bacteria cultures, mackinawite was observed almost exclusively (Ivarson and Hallberg, 1976;Neal et al, 2001;Williams et al, 2005;Ikogou et al, 2017;Stanley and Southam, 2018) and sometimes in association with greigite (Zhou et al, 2014;Picard et al, 2018). Pyrite formation in pure sulfate-reducing bacteria cultures was reported in only a single instance (Rickard, 1969b).…”

Section: Introductionmentioning

confidence: 99%

Mechanisms of Pyrite Formation Promoted by Sulfate-Reducing Bacteria in Pure Culture

et al. 2020

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Pyrite, or iron disulfide, is the most common sulfide mineral on the Earth's surface and is widespread through the geological record. Because sulfides are mainly produced by sulfate-reducing bacteria (SRB) in modern sedimentary environments, microorganisms are assumed to drive the formation of iron sulfides, in particular, pyrite. However, the exact role played by microorganisms in pyrite formation remains unclear and, to date, the precipitation of pyrite in microbial cultures has only rarely been achieved. The present work relies on chemical monitoring, electron microscopy, X-ray diffraction, and synchrotron-based spectroscopy to evaluate the formation of iron sulfides by the sulfate-reducing bacteria Desulfovibrio desulfuricans as a function of the source of iron, either provided as dissolved Fe 2+ or as Fe III-phosphate nanoparticles. Dissolved ferrous iron led to the formation of increasingly crystalline mackinawite (FeS) with time, encrusting bacterial cell walls, hence preventing further sulfate reduction upon day 5 and any evolution of iron sulfides into more stable phases, e.g., pyrite. In contrast, ferric phosphate was transformed into a mixture of large flattened crystals of well-crystallized vivianite (Fe 3 (PO 4) 2 • 8H 2 O) and a biofilm-like thin film of poorly crystallized mackinawite. Although being hosted in the iron sulfide biofilm, most cells were not encrusted. Excess sulfide delivered by the bacteria and oxidants (such as polysulfides) promoted the evolution of mackinawite into greigite (Fe 3 S 4) and the nucleation of pyrite spherules. These spherules were several hundreds of nanometers wide and occurred within the extracellular polymeric substance (EPS) of the biofilm after only 1 month. Altogether, the present study demonstrates that the mineral assemblage induced by the metabolic activity of sulfate-reducing bacteria strongly depends on the source of iron, which has strong implications for the interpretation of the presence of pyrite and vivianite in natural environments.

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“…Even though discrete Ni-sulfides are still precipitated in the biotic systems at [Ni] aq /[Fe] aq = 1:5, mass balance dictates that this phase contain at most 7% of the initial Ni fraction (assuming all metals precipitated, a maximum Ni/Fe ratio of 3.84 for the Nisulfides and minimum Ni/Fe ratios of 0.16 for the nanosheets). It is important to note that Ni incorporation increases the growth kinetics and thermodynamic stability of mackinawite, with potential implications to the fate of Ni and other various trace metals in natural environments (Kwon et al, 2015;Ikogou et al, 2017).…”

Section: Environmental Implicationsmentioning

confidence: 99%

“…Development of anoxic conditions below the sediment-water interface leads to the reduction of Fe-Mn-oxides and the oxidation of organic matter, prompting the release of Ni back into solution (Tribovillard et al, 2006;Weber et al, 2009;Hindersmann and Mansfeldt, 2014). In euxinic (i.e., anoxic and sulfidic) zones generated by the metabolism of sulfatereducing microbes, the released Ni can be re-sequestered either by co-precipitation with Fe-sulfides such as mackinawite (FeS) and pyrite (FeS 2 ) (Huerta-Diaz and Morse, 1992;Abraitis et al, 2004;Algeo and Maynard, 2004;Noël et al, 2015;Houben et al, 2017;Ikogou et al, 2017) or by precipitation as discrete Ni-sulfides (Ferris et al, 1987). Between these two mechanisms, co-precipitation with Fe-sulfides is typically the more important removal mechanism due to the high abundance of Fe (∼5 wt% Fe vs. 0.005 wt% Ni in Earth's upper crust; Rudnick and Gao, 2003) and the slower water exchange kinetics of Ni compared to Fe, leading to preferential Ni incorporation into the fasterprecipitating Fe-sulfides (Morse and Luther, 1999).…”

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confidence: 99%

Nanoparticulate Nickel-Hosting Phases in Sulfidic Environments: Effects of Ferrous Iron and Bacterial Presence on Mineral Formation Mechanism and Solid-Phase Nickel Distribution

et al. 2019

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Biogenic and Abiogenic Fe-Ni-Sulfide Nanoparticles Fe-S phases is primarily determined by the precipitation kinetics, and our experiments at [Ni] aq /[Fe] aq = 1:1 suggest that Ni-sulfide precipitation kinetics is comparable or higher than Fe-sulfides at this condition. Overall, our study allows for prediction on the phases and biogeochemical factors controlling Ni removal and availability in sulfidic environments.

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Long-term sequestration of nickel in mackinawite formed by Desulfovibrio capillatus upon Fe(III)-citrate reduction in the presence of thiosulfate

Cited by 26 publications

References 71 publications

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

Mechanisms of Pyrite Formation Promoted by Sulfate-Reducing Bacteria in Pure Culture

Nanoparticulate Nickel-Hosting Phases in Sulfidic Environments: Effects of Ferrous Iron and Bacterial Presence on Mineral Formation Mechanism and Solid-Phase Nickel Distribution

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