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Lookup NU author(s): Emeritus Professor Bernard Golding
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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.
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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