DNAzymes for amine and peptide lysine acylation

DNAzymes were previously identified by in vitro selection for a variety of chemical reactions, including several biologically relevant peptide modifications. However, finding DNAzymes for peptide lysine acylation is a substantial challenge. By using suitably reactive aryl ester acyl donors as the electrophiles, here we used in vitro selection to identify DNAzymes that acylate amines, including lysine side chains of DNA-anchored peptides. Some of the DNAzymes can transfer a small glutaryl group to an amino group. These results expand the scope of DNAzyme catalysis and suggest the future broader applicability of DNAzymes for sequence-selective lysine acylation of peptide and protein substrates.

Automated summary

DNAzymes were identified through in vitro selection for catalyzing acylation reactions on amine groups, including lysine side chains of DNA-anchored peptides, using suitably reactive aryl ester acyl donors as electrophiles. These findings expand the catalytic scope of DNAzymes and suggest potential broader applications for sequence-selective lysine acylation of peptides and proteins in the future.