Cited by 39Origins and Evolution of LifeSpace Science and Extraterrestrial LifeRNA and protein synthesis mechanisms

A prebiotic Krebs cycle analog generates amino acids with H2 and NH3 over nickel

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Kaur, Harpreet, Rauscher, Sophia A., Werner, Emilie, Song, Youngdong, Yi, Jing, Kazöne, Wahnyalo, Martin, William F., Tüysüz, Harun +1 more·2024·Chem

Abstract

Hydrogen (H 2 ) has powered microbial metabolism for roughly 4 billion years. The recent discovery that it also fuels geochemical analogs of the most ancient biological carbon fixation pathway sheds light on the origin of metabolism. However, it remains unclear whether H 2 can sustain more complex nonenzymatic reaction networks. Here, we show that H 2 drives the nonenzymatic reductive amination of six biological ketoacids and glyoxylate to give the corresponding amino acids in good yields using ammonium concentrations ranging from 6 to 150 mM. Catalytic amounts of nickel or ground meteorites enable these reactions at 22°C and pH 8. The same conditions promote an H 2 -dependent ketoacid-forming reductive aldol chemistry that co-occurs with reductive amination, producing a continuous reaction network resembling amino acid synthesis in the metabolic core of ancient microbes. The results support the hypothesis that the earliest biochemical networks could have emerged without enzymes or RNA.

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Crossref · 10.1016/j.chempr.2024.02.001

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  • Ni0 readily forms amino acids from 2-oxoacids, NH3 and H2.

    “Furthermore, Ni0 readily forms amino acids from 2‐oxoacids, NH3 and H2 [77]”
  • The same metal catalysts that allow the acetyl-CoA pathway to unfold without ATP, enzymes, or cofactors convert 2-oxoacids to amino acids at room temperature, reduce NAD+, and reduce ferredoxin with H2.

    “the same metal catalysts that allow it to unfold without ATP, enzymes, or cofactors convert 2‐oxoacids to amino acids at room temperature [77], reduce NAD+ [127] and reduce ferredoxin with H2 [79].”
  • 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 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].”

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References 71 · Cited by 39

Authors
Kaur, H., Rauscher, S. A., Werner, E., Song, Y., Yi, J., Kazöne, W., Martin, W. F., Tüysüz, H., & Moran, J.
Affiliations
  • Centre National de la Recherche Scientifique (FR)
  • Max-Planck-Institut für Kohlenforschung (DE)
  • Heinrich Heine University Düsseldorf (DE)
Corresponding author
Moran, Joseph
Venue
Chem
Publisher
Elsevier BV
Published
2024-05
Volume
10
Issue
5
Pages
1528-1540
ISSN
2451-9294 (ISSN-L)
OpenAlex
W4392203301
Cited by
39
References
71
Citations by year
2026: 15 · 2025: 11 · 2024: 13
FWCI
7.34
Type
journal article
Language
en
Open access
Locations
  • Chem (publishedVersion, cc-by-nc-nd)
  • PubMed (publishedVersion)
  • PubMed Central (acceptedVersion, cc-by-nc-nd)
  • HAL (submittedVersion, cc-by)
Funders
  • European Research Council
  • Horizon 2020 Marie Skłodowska-Curie Actions
  • Volkswagen Foundation
Topics
  • Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
  • Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Space Science and Extraterrestrial Life
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › RNA and protein synthesis mechanisms
Keywords
origin of metabolism, prebiotic chemistry, hydrogen energy, reductive amination, reductive aldol reaction, amino acid synthesis, nickel catalysis, keto acids, glyoxylic acid, origin of life

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