Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering , East China Normal University , 500 Dongchuan Road , Shanghai , 200241 , P. R. China.
Division of Physical Biology & Bioimaging Center, Shanghai Synchrotron Radiation Facility , Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800 , P. R. China.
ACS Nano. 2018 Jul 24;12(7):7093-7099. doi: 10.1021/acsnano.8b02864. Epub 2018 Jun 22.
The programmable regulation of chemical reaction networks (CRNs) represents a major challenge toward the development of complex molecular devices performing sophisticated motions and functions. Nevertheless, regulation of artificial CRNs is generally energy- and time-intensive as compared to natural regulation. Inspired by allosteric regulation in biological CRNs, we herein develop an intramolecular conformational motion strategy (InCMS) for programmable regulation of DNA CRNs. We design a DNA switch as the regulatory element to program the distance between the toehold and branch migration domain. The presence of multiple conformational transitions leads to wide-range kinetic regulation spanning over 4 orders of magnitude. Furthermore, the process of energy-cost-free strand exchange accompanied by conformational change discriminates single base mismatches. Our strategy thus provides a simple yet effective approach for dynamic programming of complex CRNs.
可编程调控化学反应网络（CRNs）是开发执行复杂运动和功能的复杂分子器件的主要挑战。然而，与自然调控相比，人工 CRNs 的调控通常需要耗费大量的能量和时间。受生物 CRNs 别构调控的启发，我们在此开发了一种用于可编程调控 DNA CRNs 的分子内构象运动策略（InCMS）。我们设计了一个 DNA 开关作为调控元件，以编程衔接区域和分支迁移区域之间的距离。多个构象转变的存在导致跨越 4 个数量级的宽范围动力学调控。此外，伴随构象变化的无能量成本的链交换过程可区分单碱基错配。因此，我们的策略为复杂 CRNs 的动态编程提供了一种简单而有效的方法。
