Synergistic Effects of Silica‐Supported Iron−Cobalt Catalysts for CO 2 Reduction to Prebiotic Organics
Open accessAbstract
To test the ability of geochemical surfaces in serpentinizing hydrothermal systems to catalyze reactions from which metabolism arose, we investigated H 2 ‐dependent CO 2 reduction toward metabolic intermediates over silica‐supported Co−Fe catalysts. Supported catalysts converted CO 2 to various products at 180 °C and 2.0 MPa. The liquid product phase included formate, acetate, and ethanol, while the gaseous product phase consisted of CH 4 , CO, methanol, and C 2 −C 7 linear hydrocarbons. The 1/1 ratio CoFe alloy with the same composition as the natural mineral wairauite yielded the highest concentrations of formate (6.0 mM) and acetate (0.8 mM), which are key intermediates in the acetyl‐coenzyme A (acetyl‐CoA) pathway of CO 2 fixation. While Co‐rich catalysts were proficient at hydrogenation, yielding mostly CH 4 , Fe‐rich catalysts favored the formation of CO and methanol. Mechanistic studies indicated intermediate hydrogenation and C−C coupling activities of alloyed CoFe, in contrast to physical mixtures of both metals. Co in the active site of Co−Fe catalysts performed a similar reaction as tetrapyrrole‐coordinated Co in the corrinoid iron‐sulfur (CoFeS) methyl transferase in the acetyl‐CoA pathway. In a temperature range characteristic for deeper regions of serpentinizing systems, oxygenate product formation was favored at lower, more biocompatible temperatures.
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Fe0, Ni0, Ni3Fe and silica-supported Co-Fe alloys can replace the proteins that synthesize formate, acetate, pyruvate from H2 and CO2 via the acetyl-CoA pathway.
“Second, Fe0, Ni0, Ni3Fe and silica‐supported Co‐Fe alloys can replace the proteins that synthesize formate, acetate, pyruvate from H2 and CO2 via the acetyl‐CoA pathway [60, 61, 62, 63, 64] (Fig. 1C).”
From Evidence for corrin biosynthesis in the last universal common ancestor (2025) · cites this paper as [64]
The Results (Prebiotic Carbon Compounds in the Liquid Phase; page unavailable) report that silica-supported Co–Fe catalysts produced formate and acetate from CO₂, and the Conclusions describe a similarity to an enzyme in the acetyl-CoA pathway. The paper does not report pyruvate production by those catalysts or establish that they replace the pathway’s proteins. Its Introduction discusses Fe- and Ni-based catalysts as earlier studies, not as catalysts tested here. (LLM, conf=0.89)
Experimental — accuracy not yet measuredThe present findings trace corrinoids to the earliest phases of biochemical evolution, to a time when some essential biochemical functions were performed by proteins, some by cofactors alone and some by solid-state metals.
“The present findings trace corrinoids to the earliest phases of biochemical evolution, to a time when some essential biochemical functions were performed by proteins, some were performed by cofactors alone and some were still performed by solid‐state metals [62, 64, 77, 90].”
From Evidence for corrin biosynthesis in the last universal common ancestor (2025) · cites this paper as [64]
The Introduction (page not available) describes metal minerals as possible prebiotic catalysts and geochemical ancestors of enzymes and cofactors. The Conclusions (page not available) link a Co–Fe mineral catalyst to a corrinoid-containing enzyme in an ancient CO₂-fixation pathway. The paper does not establish a phase in which proteins, cofactors acting alone, and solid-state metals each performed essential biochemical functions. (LLM, conf=0.84)
Experimental — accuracy not yet measuredOnly the acetyl-CoA pathway operates in vitro to form formate, acetate and pyruvate from H2 and CO2 without enzymes or cofactors, using only metals or minerals that occur in hydrothermal vents as catalysts.
“Moreover, only one of those seven, again only the acetyl CoA pathway, operates in vitro to form its main products – formate, acetate and pyruvate [49, 90] – from H2 and CO2 without enzymes or cofactors, using only metals or minerals that occur in hydrothermal vents as catalysts [60, 61, 62, 63, 64, 125].”
From Evidence for corrin biosynthesis in the last universal common ancestor (2025) · cites this paper as [64]
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Mrnjavac, N., Hoffmann, N. K., Schlikker, M. L., Burmeister, M., Schwander, L., Garcia, C. G., Brabender, M., Steel, M., Huson, D., Metzger, S., et al. (2025) · Science Advances · doi:10.1126/sciadv.aef3128 · Cited by 4 · see citing works
Self-citationWang, K., Liu, T., Hai, P., Fujii, S., Liu, C., Song, H., Zhu, C., Liu, G., Zhang, J., Wang, Z., et al. (2026) · Chemical Science · doi:10.1039/d5sc08926c · Cited by 3 · see citing works
Yang, J., Wang, K., Ding, H. Q., Li, H., Liu, Y., Liang, J., Song, W., Reubroycharoen, P., Duan, B., Zhang, J., et al. (2026) · ACS Catalysis · doi:10.1021/acscatal.6c00142 · Cited by 2 · see citing works
Prebiotic aqueous reactions catalyzed by native nickel without hydrogen
Garcia, C. G., Brabender, M., & Martin, W. F. (2026) · bioRxiv · doi:10.1111/febs.70556 · Cited by 4 · see citing works
Self-citationZhao, Y., Dummer, N., Aggett, K. J., Hutchings, G. J., Martin, W. F., & Tüysüz, H. (2026) · Advanced Synthesis & Catalysis · doi:10.1002/adsc.70531 · Cited by 2 · see citing works
Self-citationShiny metal catalysts at the origin of metabolism
Martin, W. F., Hoffmann, N. K., & Schlikker, M. L. (2026) · Trends in Microbiology · doi:10.1016/j.tim.2026.07.012 · Cited by 2 · see citing works
Self-citationLv, Z., Wang, Y., & Wang, Y. (2026) · The Innovation Life · doi:10.59717/j.xinn-life.2026.100235
- Authors
- Belthle, K. S., Martin, W. F., & Tüysüz, H.
- Affiliations
- Max-Planck-Institut für Kohlenforschung (DE)
- Heinrich Heine University Düsseldorf (DE)
- Corresponding author
- Tüysüz, Harun
- Venue
- ChemCatChem
- Publisher
- Wiley
- Published
- 2024-03-14
- Volume
- 16
- Issue
- 11
- ISSN
- 1867-3880 (ISSN-L)
- 1867-3899
- PMC
- PMC7616659
- OpenAlex
- W4391926511
- Cited by
- 12
- References
- 75
- Citations by year
- 2026: 7 · 2024: 5
- FWCI
- 2.26
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- ChemCatChem (publishedVersion, cc-by-nc)
- PubMed (publishedVersion)
- PubMed Central (acceptedVersion, cc-by-nc-nd)
- Funders
- Volkswagen Foundation (96_742)
- Deutsche Forschungsgemeinschaft (MA-1426/21-1/TU 315/8-1)
- Topics
- Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
- 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
- CO2 reduction, prebiotic chemistry, silica-supported catalysts, Fe-Co alloys, serpentinization, hydrothermal systems, origin of metabolism, acetyl-CoA pathway, formate, acetate, hydrogenation, C–C coupling, CO2 fixation
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