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Cited by 41Catalysts for Methane ReformingCarbon dioxide utilization in catalysisCO2 Reduction Techniques and Catalysts

Effects of Silica Modification (Mg, Al, Ca, Ti, and Zr) on Supported Cobalt Catalysts for H2-Dependent CO2 Reduction to Metabolic Intermediates

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Belthle, Kendra S., Beyazay, Tuğçe, Ochoa-Hernández, Cristina, Miyazaki, Ray, Foppa, Lucas, Martin, William F., Tüysüz, Harun·2022·Journal of the American Chemical Society
DOI 10.1021/jacs.2c08845PMC PMC9706562
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Abstract

fixation, in line with the idea that autotrophic metabolism emerged at hydrothermal vents.

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  • Under the conditions of serpentinizing hydrothermal vents, transition metals alone convert H2 and CO2 into formate, acetate and pyruvate in water.

    “Under the conditions of serpentinizing hydrothermal vents, transition metals alone convert H2 and CO2 into formate, acetate and pyruvate in water [60, 62, 63, 158].”

    From Evidence for corrin biosynthesis in the last universal common ancestor (2025) · cites this paper as [158]

    The Introduction reports that Fe- and Ni-based catalysts produce formate, acetate, and pyruvate from H2 and CO2 under simulated hydrothermal-vent conditions. But this paper’s own cobalt experiments produced formate and acetate, not pyruvate, and its Results describe a fixed-bed reaction under reduced water activity rather than conversion in water (page numbers unavailable). (LLM, conf=0.85)

    Experimental — accuracy not yet measured

  • Vent reactions were promoted by inorganic catalysts, likely including greigite (Fe3S4), magnetite (Fe3O4), and awaruite (Ni3Fe), as well as heteroatoms incorporating Co, Mg, Al, Ca, Ti, and Zr, in the vent flux and microchamber walls.

    “Vent reactions were promoted by inorganic catalysts, likely including greigite (Fe3S4), magnetite (Fe3O4), and awaruite (Ni3Fe), as well as heteroatoms incorporating Co, Mg, Al, Ca, Ti, and Zr, in the vent flux and microchamber walls [98,99,100].”

    From Opinion: The Key Steps in the Origin of Life to the Formation of the Eukaryotic Cell (2024) · cites this paper as [98]

    The Introduction (page not available) describes transition-metal catalysis at hydrothermal vents and says the authors selected Mg, Al, Ca, Ti, and Zr based on cations in vent minerals. The Results (page not available) demonstrate CO₂ hydrogenation using laboratory-made cobalt catalysts on modified silica supports. The paper does not identify greigite, magnetite, or awaruite as the catalysts in question, or establish that these cobalt-containing materials promoted reactions in actual vent flux or microchamber walls. (LLM, conf=0.87)

    Experimental — accuracy not yet measured

  • Formate formation under serpentinizing conditions can be replicated in the laboratory, where formate is typically the most abundant reduced carbon species under a variety of conditions.

    “This can also be replicated in the laboratory (Preiner et al., 2020), where formate is typically the most abundant reduced carbon species under a variety of conditions (Belthle et al., 2022; Beyazay et al., 2023a,b).”

    From Serpentinization as the source of energy, electrons, organics, catalysts, nutrients and pH gradients for the origin of LUCA and life (2023) · cites this paper as Belthle et al., 2022

    The Results section (page not available) reports laboratory formation of formate with several cobalt catalysts; among the measured liquid-phase oxygenates, its concentration exceeded acetate’s across the supports compared. But the Results also state that methane was the main product for all modified-support catalysts, so the paper does not support calling formate the most abundant reduced carbon species overall under a variety of conditions. The separate laboratory-replication clause is cited to Preiner et al., not to this source. (LLM, conf=0.88)

    Experimental — accuracy not yet measured

  • Metals (Fe, Ni, Co) and metal oxides can serve as hydrogenases, activating H2 by splitting it into two metal bound hydrogen atoms for CO2 reduction or for NAD+ reduction.

    “Metals (Fe, Ni, Co) and metal oxides can serve as hydrogenases, activating H2 by splitting it into two metal bound hydrogen atoms for CO2 reduction (Preiner et al., 2020; Belthle et al., 2022; Beyazay et al., 2023a,b) or for NAD+ reduction (Henriques Pereira et al., 2022).”

    From Serpentinization as the source of energy, electrons, organics, catalysts, nutrients and pH gradients for the origin of LUCA and life (2023) · cites this paper as Belthle et al., 2022

    The Introduction describes Fe- and Ni-based catalysts for H₂-dependent CO₂ fixation, and the Conclusion reports that supported Co nanoparticles catalyze CO₂ hydrogenation (page numbers unavailable). The cited paper does not establish that these materials serve as hydrogenases or activate H₂ by splitting it into two metal-bound hydrogen atoms. The NAD⁺ reduction clause is attributed to a different citation, not this paper. (LLM, conf=0.88)

    Experimental — accuracy not yet measured

  • The synthesis of formate, acetate and pyruvate from H2 and CO2 under simulated hydrothermal conditions using Ni3Fe or Fe3O4 as catalysts requires no participation of sulfur.

    “Note however that the synthesis of formate, acetate and pyruvate from H2 and CO2 under simulated hydrothermal conditions using Ni3Fe or Fe3O4 as catalysts requires no participation of sulfur (Preiner et al., 2020; Belthle et al., 2022; Beyazay et al., 2023a,b).”

    From Serpentinization as the source of energy, electrons, organics, catalysts, nutrients and pH gradients for the origin of LUCA and life (2023) · cites this paper as Belthle et al., 2022

    The Introduction (page not provided) reports that Fe- and Ni-based catalysts produce formate, acetate, and pyruvate from H2 and CO2 under simulated hydrothermal conditions. It does not identify Ni3Fe or Fe3O4 as the catalysts or state that sulfur is unnecessary; this paper's own experiments instead use supported cobalt catalysts. (LLM, conf=0.84)

    Experimental — accuracy not yet measured

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Cited by

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Authors
Belthle, K. S., Beyazay, T., Ochoa-Hernández, C., Miyazaki, R., Foppa, L., Martin, W. F., & Tüysüz, H.
Affiliations
  • Max-Planck-Institut für Kohlenforschung (DE)
  • Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470 Mülheim an der Ruhr, Germany
  • Fritz Haber Institute of the Max Planck Society (DE)
  • Heinrich Heine University Düsseldorf (DE)
Corresponding author
Tüysüz, Harun
ORCID
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2022-11-09
Volume
144
Issue
46
Pages
21232-21243
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/jacs.2c08845
PMC
PMC9706562
OpenAlex
W4308633833
Cited by
41
References
10
Citations by year
2026: 6 · 2025: 7 · 2024: 17 · 2023: 10 · 2022: 1
FWCI
1.58
Type
journal article
Language
en
Open access
Licence
Locations
  • Journal of the American Chemical Society (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
Funders
  • Deutsche Forschungsgemeinschaft (MA-1426/21-1 / TU 315/8-1)
  • Max-Planck-Gesellschaft
  • Volkswagen Foundation (96_742)
Topics
  • Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
  • Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
supported cobalt catalysts, CO2 reduction, metabolic intermediates, silica modification, magnesium, aluminum, calcium, titanium, zirconium, autotrophic metabolism, hydrothermal vents, CO2 fixation
MeSH terms
Acetates, Carbon Dioxide, Cobalt, Formates, Oxides, Silicon Dioxide, Titanium

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