Department of Chemistry, Tulane University, 2015 Percival Stern Hall, New Orleans, Louisiana 70118, United States.
Department of Chemistry, Xavier University of Louisiana, 1 Drexel Drive, New Orleans, Louisiana 70125, United States.
J Am Chem Soc. 2022 Sep 14;144(36):16502-16511. doi: 10.1021/jacs.2c05726. Epub 2022 Sep 5.
Base-pair-driven toehold-mediated strand displacement (BP-TMSD) is a fundamental concept employed for constructing DNA machines and networks with a gamut of applications─from theranostics to computational devices. To broaden the toolbox of dynamic DNA chemistry, herein, we introduce a synthetic surrogate termed host-guest-driven toehold-mediated strand displacement (HG-TMSD) that utilizes bioorthogonal, cucurbit[7]uril (CB[7]) interactions with guest-linked input sequences. Since control of the strand-displacement process is salient, we demonstrate how HG-TMSD can be finely modulated via changes to the structure of the input sequence (including synthetic guest head-group and/or linker length). Further, for a given input sequence, competing small-molecule guests can serve as effective regulators (with fine and coarse control) of HG-TMSD. To show integration into functional devices, we have incorporated HG-TMSD into machines that control enzyme activity and layered reactions that detect specific microRNA.
碱基对驱动的引发链置换（BP-TMSD）是构建具有广泛应用的 DNA 机器和网络的基本概念，从治疗到计算设备。为了拓宽动态 DNA 化学的工具包，在此，我们引入了一种称为主体-客体驱动的引发链置换（HG-TMSD）的合成替代物，它利用了生物正交的葫芦[7]脲（CB[7]）与连接客体的输入序列的相互作用。由于对链置换过程的控制至关重要，我们展示了如何通过改变输入序列的结构（包括合成客体头部基团和/或连接体长度）来精细调节 HG-TMSD。此外，对于给定的输入序列，竞争的小分子客体可以作为 HG-TMSD 的有效调节剂（具有精细和粗调控制）。为了展示集成到功能设备中，我们已经将 HG-TMSD 整合到控制酶活性的机器和检测特定 microRNA 的层状反应中。
