Triplet-Encoded Prebiotic RNA Aminoacylation

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Su, Meng; orcid: 0000-0001-6558-8712; paragon-plus: 5579267 
Schmitt, Christian; paragon-plus: 6603134 
Liu, Ziwei; paragon-plus: 4131200; orcid: 0000-0002-1812-2538 
Roberts, Samuel J.; paragon-plus: 5897191; orcid: 0000-0002-7324-7325 
Liu, Kim C.; paragon-plus: 6603137 

The encoding step of translation involves attachment of amino acids to cognate tRNAs by aminoacyl-tRNA synthetases, themselves the product of coded peptide synthesis. So, the question arisesbefore these enzymes evolved, how were primordial tRNAs selectively aminoacylated? Here, we demonstrate enzyme-free, sequence-dependent, chemoselective aminoacylation of RNA. We investigated two potentially prebiotic routes to aminoacyl-tRNA acceptor stem-overhang mimics and analyzed those oligonucleotides undergoing the most efficient aminoacylation. Overhang sequences do not significantly influence the chemoselectivity of aminoacylation by either route. For aminoacyl-transfer from a mixed anhydride donor strand, the chemoselectivity and stereoselectivity of aminoacylation depend on the terminal three base pairs of the stem. The results support early suggestions of a second genetic code in the acceptor stem.

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Journal of the American Chemical Society
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American Chemical Society
Simons Foundation (290362)
Medical Research Council (MC_UP_A024_1009)
P11 , Deutsche Forschungsgemeinschaft (CRC)