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  Role of geochemical protoenzymes (geozymes) in primordial metabolism: specific abiotic hydride transfer by metals to the biological redox cofactor NAD+

Henriques Pereira, D. P., Leethaus, J., Beyazay, T., do Nascimento, A., Kleinermanns, K., Tüysüz, H., et al. (2021). Role of geochemical protoenzymes (geozymes) in primordial metabolism: specific abiotic hydride transfer by metals to the biological redox cofactor NAD+. The FEBS Journal. doi:10.1111/febs.16329.

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 Creators:
Henriques Pereira, Delfina P.1, Author
Leethaus, Jana1, Author
Beyazay, Tugce2, Author              
do Nascimento, Andey1, Author
Kleinermanns, Karl3, Author
Tüysüz, Harun2, Author              
Martin, William F.1, Author
Preiner, Martina4, 5, Author
Affiliations:
1Institute for Molecular Evolution, Heinrich Heine University, Düsseldorf, Germany, ou_persistent22              
2Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950290              
3Institute for Physical Chemistry, Heinrich Heine University, Düsseldorf, Germany, ou_persistent22              
4Department of Ocean Systems, Royal Netherlands Institute for Sea Research, Den Burg, The Netherlands, ou_persistent22              
5Department of Earth Sciences, Utrecht University, The Netherlands, ou_persistent22              

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Free keywords: cofactors; electron donors; hydrogen; hydrogenase; NADH; origin of life; reduction; serpentinizing systems
 Abstract: Hydrogen gas, H2, is generated in serpentinizing hydrothermal systems, where it has supplied electrons and energy for microbial communities since there was liquid water on Earth. In modern metabolism, H2 is converted by hydrogenases into organically bound hydrides (H), for example, the cofactor NADH. It transfers hydrides among molecules, serving as an activated and biologically harnessed form of H2. In serpentinizing systems, minerals can also bind hydrides and could, in principle, have acted as inorganic hydride donors—possibly as a geochemical protoenzyme, a ‘geozyme’— at the origin of metabolism. To test this idea, we investigated the ability of H2 to reduce NAD+ in the presence of iron (Fe), cobalt (Co) and nickel (Ni), metals that occur in serpentinizing systems. In the presence of H2, all three metals specifically reduce NAD+ to the biologically relevant form, 1,4-NADH, with up to 100% conversion rates within a few hours under alkaline aqueous conditions at 40 °C. Using Henry's law, the partial pressure of H2 in our reactions corresponds to 3.6 mm, a concentration observed in many modern serpentinizing systems. While the reduction of NAD+ by Ni is strictly H2-dependent, experiments in heavy water (2H2O) indicate that native Fe can reduce NAD+ both with and without H2. The results establish a mechanistic connection between abiotic and biotic hydride donors, indicating that geochemically catalysed, H2-dependent NAD+ reduction could have preceded the hydrogenase-dependent reaction in evolution.

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Language(s): eng - English
 Dates: 2021-11-182021-12-172021-12-18
 Publication Status: Published online
 Pages: 15
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1111/febs.16329
 Degree: -

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Title: The FEBS Journal
  Other : The Federation if European Biochemical Societies Journal
Source Genre: Journal
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Publ. Info: Wiley-Blackwell
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 1742-464X
CoNE: https://pure.mpg.de/cone/journals/resource/954925398485