Abstract

3′,5′-Cyclic GMP spontaneously nonenzymatically polymerizes in a base-catalyzed reaction affording G oligonucleotides. When reacted with fully or partially sequence-complementary RNA (oligo C), the abiotically generated oligo G RNA displays a typical ribozyme activity consisting of terminal ligation accompanied by cleavage of an internal phosphate site of the donor oligonucleotide stem upon attack of the acceptor 3′ terminal OH. This reaction is dubbed Ligation following Intermolecular Cleavage (LIC). In a prebiotic perspective, the ability of oligo G polynucleotides to react with other sequences outlines a simple and possible evolutionary scenario based on the autocatalytic properties of RNA.

Highlights

  • In the quest for the initialgenetic materials, the autocatalytic potential of RNA [1,2,3,4,5,6] remains unmatched

  • For the theoretical description of the ligation reaction we considered a model consisting of a donor guanosine-phosphate nucleotide and an acceptor cytidine, which were stabilized by interbase stacking

  • The studied RNA molecules deriving from the interactions of nonenzymatically polymerized oligoG with oligonucleotides containing a sufficiently long complementary sequence are active ribozymes

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Summary

Introduction

In the quest for the initial (pre)genetic materials, the autocatalytic potential of RNA [1,2,3,4,5,6] remains unmatched. RNA provides, for the time being, the only plausible solution to self-generation, as allowed by self-polymerization and by a variety of self-catalytic processes. Pioneering reports of RNA recombination have appeared [7,8,9,10,11,12]. With the possible exception of the systems described in [13,14,15], the reactions reported so far are not simple and robust enough to be of likely prebiotic relevance. The reaction is low yielding, but it shows that, inefficient, RNA may generate itself from prebiotic precursors [18,19,20]. Efficient enzyme-free copying of all four pre-activated nucleobases, templated by immobilized RNA, was reported [24]

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