Department of Chemistry, Simon Fraser University, Burnaby, British Columbia V5A 1S6, Canada.
Department of Molecular Biology and Biochemistry, Simon Fraser University, Burnaby, British Columbia V5A 1S6, Canada.
Langmuir. 2024 Oct 1;40(39):20576-20583. doi: 10.1021/acs.langmuir.4c02314. Epub 2024 Sep 21.
We have systematically investigated and found surprising superior catalytic activities of very short DNAzymes for copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC), both in solution and on surface. As a key reaction of the "click chemistry" class, CuAAC is a highly efficient and specific covalent conjugation tool with demonstrated applications in organic synthesis, bioconjugation, and surface functionalization; however, it requires the presence of the Cu(I) catalyst, which is an unstable species in aqueous solutions. We show here that one ultrashort, 14-nucleotide-truncated fragment of an earlier selected DNAzyme (CLICK-17) shows a striking and superior catalytic activity toward the CuAAC reaction in solution and on surface in the presence of either Cu(I) or Cu(II), at significantly lowered concentrations. These results obviate the need for long-sequence DNAzymes, selected out of the homogeneous solution phase, for application in complex surface environments.
我们已经系统地研究并发现非常短的 DNA 酶在铜(I)催化的叠氮-炔环加成(CuAAC)反应中具有惊人的优越催化活性,无论是在溶液中还是在表面上。作为“点击化学”类的关键反应,CuAAC 是一种高效且特异性的共价偶联工具,已在有机合成、生物缀合和表面功能化中得到证实;然而,它需要存在 Cu(I)催化剂,而 Cu(I)催化剂在水溶液中是一种不稳定的物质。我们在这里展示,一个经过早期选择的 DNA 酶(CLICK-17)的 14 个核苷酸截断片段在存在 Cu(I)或 Cu(II)的情况下,在溶液中和表面上均表现出对 CuAAC 反应的惊人和优越的催化活性,所需浓度显著降低。这些结果消除了在复杂表面环境中应用时对从均相溶液相中筛选出的长序列 DNA 酶的需求。