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Record W4405616589 · doi:10.1111/febs.17357

Conversion of pyridoxal to pyridoxamine with <scp>NH</scp> <sub>3</sub> and <scp>H</scp> <sub>2</sub> on nickel generates a protometabolic nitrogen shuttle under serpentinizing conditions

2024· article· en· W4405616589 on OpenAlexaff
Manon Laura Schlikker, Max Brabender, Loraine Schwander, Carolina García García, M. Burmeister, Sabine Metzger, Joseph Moran, William Martin

Bibliographic record

VenueFEBS Journal · 2024
Typearticle
Languageen
FieldPhysics and Astronomy
TopicOrigins and Evolution of Life
Canadian institutionsUniversity of Ottawa
FundersVolkswagen FoundationH2020 European Research CouncilDeutsche ForschungsgemeinschaftEuropean Commission
KeywordsTransaminationPyridoxamineChemistryCatalysisPyridoxalAmino acidNickelStereochemistryEnzymeMedicinal chemistryBiochemistryOrganic chemistry

Abstract

fetched live from OpenAlex

Serpentinizing hydrothermal vents are likely sites for the origin of metabolism because they produce H 2 as a source of electrons for CO 2 reduction while depositing zero‐valent iron, cobalt, and nickel as catalysts for organic reactions. Recent work has shown that solid‐state nickel can catalyze the H 2 ‐dependent reduction of CO 2 to various organic acids and their reductive amination with H 2 and NH 3 to biological amino acids under the conditions of H 2 ‐producing hydrothermal vents and that amino acid synthesis from NH 3 , H 2 , and 2‐oxoacids is facile in the presence of Ni 0 . Such reactions suggest a metallic origin of metabolism during early biochemical evolution because single metals replace the function of over 130 enzymatic reactions at the core of metabolism in microbes that use the acetyl‐CoA pathway of CO 2 fixation. Yet solid‐state catalysts tether primordial amino synthesis to a mineral surface. Many studies have shown that pyridoxal catalyzes transamination reactions without enzymes. Here we show that pyridoxamine, the NH 2 ‐transferring intermediate in pyridoxal‐dependent transamination reactions, is generated from pyridoxal by reaction with NH 3 (as little as 5 m m ) and H 2 (5 bar) on Ni 0 as catalyst at pH 11 and 80 °C within hours. These conditions correspond to those in hydrothermal vents undergoing active serpentinization. The results indicate that at the origin of metabolism, pyridoxamine provided a soluble, organic amino donor for aqueous amino acid synthesis, mediating an evolutionary transition from NH 3 ‐dependent amino acid synthesis on inorganic surfaces to pyridoxamine‐dependent organic reactions in the aqueous phase.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.092
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0010.001
Science and technology studies0.0010.000
Scholarly communication0.0000.001
Open science0.0000.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.012
GPT teacher head0.241
Teacher spread0.229 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations8
Published2024
Admission routes1
Has abstractyes

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