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Cited by 52Origins and Evolution of LifeRNA and protein synthesis mechanismsEarth Systems and Cosmic Evolution

Elements of Metabolic Evolution

Huber, Claudia, Kraus, Florian, Hanzlik, Marianne, Eisenreich, Wolfgang, Wächtershäuser, Günter·2012·Chemistry – A European Journal
DOI 10.1002/chem.201102914
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Abstract

Research into the origin of evolution is polarized between a genetics‐first approach, with its focus on polymer replication, and a metabolism‐first approach that takes aim at chemical reaction cycles. Taking the latter approach, we explored reductive carbon fixation in a volcanic hydrothermal setting, driven by the chemical potential of quenched volcanic fluids for converting volcanic C1 compounds into organic products by transition‐metal catalysts. These catalysts are assumed to evolve by accepting ever‐new organic products as ligands for enhancing their catalytic power, which in turn enhances the rates of synthetic pathways that give rise to ever‐new organic products, with the overall effect of a self‐expanding metabolism. We established HCN, CO, and CH 3 SH as carbon nutrients, CO and H 2 as reductants, and iron‐group transition metals as catalysts. In one case, we employed the “cyano‐system” [Ni(OH)(CN)] with [Ni(CN)4]2− as the dominant nickel–cyano species. This reaction mainly produced α‐amino acids and α‐hydroxy acids as well as various intermediates and derivatives. An organo‐metal‐catalyzed mechanism is suggested that mainly builds carbon skeletons by repeated cyano insertions, with minor CO insertions in the presence of CO. The formation of elemental nickel (Ni 0) points to an active reduced‐nickel species. In another case, we employed the mercapto–carbonyl system [Co 2(CO)8]/Ca(OH)2/CO for the double‐carbonylation of mercaptans. In a “hybrid system”, we combined benzyl mercaptan with the cyano system, in which [Ni(OH)(CN)] was the most productive for the double‐carbon‐fixation reaction. Finally, we demonstrated that the addition of products of the cyano system (Gly, Ala) to the hybrid system increased productivity. These results demonstrate the chemical possibility of metabolic evolution through rate‐promotion of one synthetic reaction by the products of another.

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  • Enzymes of core carbon and energy pathways in modern anaerobic autotrophs are replete with FeS, FeNiS and MoS (WS) centres.

    “This is an important similarity to modern anaerobic autotrophs, whose enzymes of core carbon and energy pathways are replete with FeS, FeNiS and MoS (WS) centres, FeS and NiS usually being incorporated into proteins via cysteine residues [54–58], Mo and W usually being complexed by thiols of the molybdopterin cofactor MoCo [59].”

    From Early bioenergetic evolution (2013) · cites this paper as [55]

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Authors
Huber, C., Kraus, F., Hanzlik, M., Eisenreich, W., & Wächtershäuser, G.
Affiliations
Technical University of Munich (DE)
Corresponding author
  • Eisenreich, Wolfgang
  • Wächtershäuser, Günter
ORCID
Venue
Chemistry – A European Journal
Publisher
Wiley
Published
2012-01-13
Volume
18
Issue
7
Pages
2063-2080
ISSN
  • 0947-6539 (ISSN-L)
  • 1521-3765
DOI
10.1002/chem.201102914
OpenAlex
W2007101531
Cited by
52
References
13
Citations by year
2026: 3 · 2024: 4 · 2023: 1 · 2022: 2 · 2021: 6 · 2020: 3 · 2019: 3 · 2018: 1 · 2017: 4 · 2016: 3 · 2015: 1 · 2014: 6 · 2013: 11 · 2012: 4
FWCI
3.85
Type
journal article
Language
en
Open access
closed
Licence
onlinelibrary.wiley.com/termsAndConditions#vor (vor)
Locations
  • Chemistry - A European Journal (publishedVersion)
  • PubMed (publishedVersion)
Topics
  • Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › RNA and protein synthesis mechanisms
  • Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Earth Systems and Cosmic Evolution
Keywords
origin of metabolism, metabolic evolution, hydrothermal systems, transition metal catalysis, nickel cyanide, cobalt carbonyl, benzyl mercaptan, α-amino acids, α-hydroxy acids, organic synthesis, volcanic fluids, prebiotic chemistry
MeSH terms
Amino Acids, Carbon, Biological Evolution, Hydroxides, Metals, Nickel, Solubility, Water, Volcanic Eruptions

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