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Non-enzymatic Ribonucleotide Reduction in the Prebiotic Context

Lookup NU author(s): Professor Bernard Golding

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Abstract

Model studies of prebiotic chemistry have revealed compelling routes for the formation of the building blocks of proteins and RNA, but not DNA. Today, deoxynucleotides required for the construction of DNA are produced by reduction of nucleotides catalysed by ribonucleotide reductases, which are radical enzymes. This study considers potential non-enzymatic routes via intermediate radicals for the ancient formation of deoxynucleotides. In this context, several mechanisms for ribonucleotide reduction, in a putative H2S/HS. environment, are characterized using computational chemistry. A bio-inspired mechanistic cycle involving a keto intermediate and HSSH production is found to be potentially viable. An alternative pathway, proceeding through an enol intermediate is found to exhibit similar energetic requirements. Non-cyclical pathways, in which HSS. is generated in the final step instead of HS., show a markedly increased thermodynamic driving force (ca. 70kJmol(-1)) and thus warrant serious consideration in the context of the prebiotic ribonucleotide reduction.


Publication metadata

Author(s): Dragicevic I, Baric D, Kovacevic B, Golding BT, Smith DM

Publication type: Article

Publication status: Published

Journal: Chemistry: A European Journal

Year: 2015

Volume: 21

Issue: 16

Pages: 6132-6143

Print publication date: 13/04/2015

Online publication date: 06/03/2015

Acceptance date: 01/01/1900

ISSN (print): 0947-6539

ISSN (electronic): 1521-3765

Publisher: Wiley - V C H Verlag GmbH & Co. KGaA

URL: http://dx.doi.org/10.1002/chem.201405741

DOI: 10.1002/chem.201405741


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