Department of Chemistry, University of Illinois Urbana-Champaign, 600 South Mathews Avenue, Urbana, IL-61801, USA.
Angew Chem Int Ed Engl. 2024 Feb 12;63(7):e202317565. doi: 10.1002/anie.202317565. Epub 2024 Jan 11.
We used in vitro selection to identify DNAzymes that acylate the exocyclic nucleobase amines of cytidine, guanosine, and adenosine in DNA oligonucleotides. The acyl donor was the 2,3,5,6-tetrafluorophenyl ester (TFPE) of a 5'-carboxyl oligonucleotide. Yields are as high as >95 % in 6 h. Several of the N-acylation DNAzymes are catalytically active with RNA rather than DNA oligonucleotide substrates, and eight of nine DNAzymes for modifying C are site-specific (>95 %) for one particular substrate nucleotide. These findings expand the catalytic ability of DNA to include site-specific N-acylation of oligonucleotide nucleobases. Future efforts will investigate the DNA and RNA substrate sequence generality of DNAzymes for oligonucleotide nucleobase N-acylation, toward a universal approach for site-specific oligonucleotide modification.
我们使用体外选择技术来鉴定能够酰化 DNA 寡核苷酸中环外核苷碱基氨基的 DNA 酶。酰基供体是 5'-羧基寡核苷酸的 2,3,5,6-四氟苯基酯 (TFPE)。在 6 小时内，产率高达>95%。几种 N-酰化 DNA 酶在 RNA 而不是 DNA 寡核苷酸底物上具有催化活性，并且 9 个用于修饰 C 的 DNA 酶中有 8 个对特定底物核苷酸具有特异性 (>95%)。这些发现扩展了 DNA 的催化能力，包括寡核苷酸碱基的特异性 N-酰化。未来的研究将调查 DNA 和 RNA 底物序列对寡核苷酸碱基 N-酰化的 DNA 酶的普遍性，以期实现通用的寡核苷酸修饰方法。
