Department of Chemistry, University of Illinois at Urbana-Champaign, 600 South Mathews Avenue, Urbana, IL 61801, USA.
Org Biomol Chem. 2021 Jan 6;19(1):171-181. doi: 10.1039/d0ob02015j.
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.
DNA 酶以前是通过体外选择来识别各种化学反应而被发现的,包括几种与生物学相关的肽修饰。然而,寻找用于肽赖氨酸酰化的 DNA 酶是一个巨大的挑战。通过使用适当反应性的芳基酯酰供体作为亲电试剂,我们在这里使用体外选择来鉴定酰化胺的 DNA 酶,包括 DNA 固定肽的赖氨酸侧链。一些 DNA 酶可以将一个小的戊二酰基转移到一个氨基上。这些结果扩展了 DNA 酶催化的范围,并表明未来 DNA 酶在肽和蛋白质底物的序列选择性赖氨酸酰化方面有更广泛的适用性。