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Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis

Hydrogen (H(2)) is a geological source of reducing electrons that is thought to have powered the metabolism of the last universal common ancestor to all extant life, and that is still metabolized by various modern organisms. It has been suggested that H(2) drove a geochemical analogue of some or all...

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Autores principales: Rauscher, Sophia A., Moran, Joseph
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10100321/
https://www.ncbi.nlm.nih.gov/pubmed/36251920
http://dx.doi.org/10.1002/anie.202212932
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author Rauscher, Sophia A.
Moran, Joseph
author_facet Rauscher, Sophia A.
Moran, Joseph
author_sort Rauscher, Sophia A.
collection PubMed
description Hydrogen (H(2)) is a geological source of reducing electrons that is thought to have powered the metabolism of the last universal common ancestor to all extant life, and that is still metabolized by various modern organisms. It has been suggested that H(2) drove a geochemical analogue of some or all of the reverse Krebs cycle at the emergence of the metabolic network, catalyzed by metals, but this has yet to be demonstrated experimentally. Herein, we show that three consecutive steps of the reverse Krebs cycle, converting oxaloacetate into succinate, can be driven without enzymes and in one‐pot by H(2) as the reducing agent under mild conditions compatible with biological chemistry. Low catalytic amounts of nickel (10–20 mol %) or platinum group metals (0.1–1 mol %) or even small amounts of ground meteorites were found to promote the reductive chemistry at temperatures between 5 and 60 °C and over a wide pH range, including pH 7. These results lend additional support to the hypothesis that geologically produced hydrogen and metal catalysts could have initiated early metabolic networks.
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spelling pubmed-101003212023-04-14 Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis Rauscher, Sophia A. Moran, Joseph Angew Chem Int Ed Engl Communications Hydrogen (H(2)) is a geological source of reducing electrons that is thought to have powered the metabolism of the last universal common ancestor to all extant life, and that is still metabolized by various modern organisms. It has been suggested that H(2) drove a geochemical analogue of some or all of the reverse Krebs cycle at the emergence of the metabolic network, catalyzed by metals, but this has yet to be demonstrated experimentally. Herein, we show that three consecutive steps of the reverse Krebs cycle, converting oxaloacetate into succinate, can be driven without enzymes and in one‐pot by H(2) as the reducing agent under mild conditions compatible with biological chemistry. Low catalytic amounts of nickel (10–20 mol %) or platinum group metals (0.1–1 mol %) or even small amounts of ground meteorites were found to promote the reductive chemistry at temperatures between 5 and 60 °C and over a wide pH range, including pH 7. These results lend additional support to the hypothesis that geologically produced hydrogen and metal catalysts could have initiated early metabolic networks. John Wiley and Sons Inc. 2022-11-22 2022-12-19 /pmc/articles/PMC10100321/ /pubmed/36251920 http://dx.doi.org/10.1002/anie.202212932 Text en © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Communications
Rauscher, Sophia A.
Moran, Joseph
Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title_full Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title_fullStr Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title_full_unstemmed Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title_short Hydrogen Drives Part of the Reverse Krebs Cycle under Metal or Meteorite Catalysis
title_sort hydrogen drives part of the reverse krebs cycle under metal or meteorite catalysis
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10100321/
https://www.ncbi.nlm.nih.gov/pubmed/36251920
http://dx.doi.org/10.1002/anie.202212932
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