Short DNAzymes for Efficient Catalysis of “Click” Reactions in Solution and on Surface

IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Tsz Yan Leung, Lin Qi, Kun Liu, Dipankar Sen, Hua-Zhong Yu
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Abstract

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 in vitro selected DNAzyme (CLICK-17) shows a striking and superior catalytic activity toward the in trans 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.
在溶液和表面高效催化 "点击 "反应的短 DNA 酶
我们对极短 DNA 酶在溶液和表面催化叠氮-炔环加成反应(CuAAC)中的催化活性进行了系统研究,结果令人惊讶。作为 "点击化学 "类的一个关键反应,CuAAC 是一种高效、特异的共价连接工具,在有机合成、生物共轭和表面功能化方面都有明显的应用;然而,它需要 Cu(I) 催化剂的存在,而 Cu(I) 催化剂在水溶液中是一种不稳定的物质。我们在此展示了早先体外筛选出的 DNA 酶(CLICK-17)的一个超短 14 核苷酸截断片段,它在 Cu(I)或 Cu(II)存在的溶液和表面中,以显著降低的浓度对反式 CuAAC 反应显示出惊人和卓越的催化活性。这些结果证明,在复杂的表面环境中应用长序列 DNA 酶时,无需从均质溶液相中进行筛选。
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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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