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Diederich, P. ; Seitz, C.* ; Buckett, L. ; Salzer, L. ; Geisberger, T.* ; Eisenreich, W.* ; Huber, C.* ; Schmitt-Kopplin, P.

Nickel-organo compounds as potential enzyme precursors under simulated early Earth conditions.

Comm. Chem. 7:33 (2024)
Verlagsversion DOI PMC
Creative Commons Lizenzvertrag
The transition from inorganic catalysis through minerals to organic catalysis by enzymes is a necessary step in the emergence of life. Our work is elucidating likely reactions at the earliest moments of Life, prior to the existence of enzymatic catalysis, by exploring essential intersections between nickel bioinorganic chemistry and pterin biochemistry. We used a prebiotically-inspired acetylene-containing volcanic hydrothermal experimental environment to shed light on the efficient formation of nickel-organo complexes. The simplest bis(dithiolene)nickel complex (C2H2S2)2Ni was identified by UV/Vis spectroscopy, mass spectrometry, nuclear magnetic resonance. Its temporal progression and possible function in this simulated early Earth atmosphere were investigated by isolating the main bis(dithiolene)nickel species from the primordial experimental setup. Using this approach, we uncovered a significant diversity of nickel-organo compositions by identifying 156 elemental annotations. The formation of acetaldehyde through the subsequent degradation of these organo-metal complexes is intriguing, as it is reminiscent of the ability of Pelobacter acetylenicus to hydrate acetylene to acetaldehyde via its bis(dithiolene)-containing enzyme acetylene hydratase. As our findings mechanistically characterize the role of nickel sulfide in catalyzing the formation of acetaldehyde, this fundamental pre-metabolic reaction could play the role of a primitive enzyme precursor of the enzymatic acetylene metabolism and further strengthen the role of acetylene in the molecular origin of life.
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Publikationstyp Artikel: Journalartikel
Dokumenttyp Wissenschaftlicher Artikel
Korrespondenzautor
Schlagwörter Delocalized Ground-states; Coordination-compounds; Acetylene; Complex; Ligand
ISSN (print) / ISBN 2399-3669
e-ISSN 2399-3669
Zeitschrift Communications Chemistry
Quellenangaben Band: 7, Heft: 1, Seiten: , Artikelnummer: 33 Supplement: ,
Verlag Springer
Verlagsort Heidelberger Platz 3, Berlin, 14197, Germany
Nichtpatentliteratur Publikationen
Begutachtungsstatus Peer reviewed
Institut(e) Research Unit Analytical BioGeoChemistry (BGC)
Förderungen Hans-Fischer-Gesellschaft
Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)
This research was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - Project-ID 364653263 - TRR 235 (CRC 235).