Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
J Am Chem Soc. 2020 Aug 26;142(34):14437-14442. doi: 10.1021/jacs.0c05669. Epub 2020 Aug 11.
Within the broad research efforts to engineer chemical pathways to yield high-throughput evolutionary synthesis of genes and their screening for dictated functionalities, we introduce the evolution of nucleic-acid-based constitutional dynamic networks (CDNs) that follow reproduction/variation/selection principles. These fundamental principles are demonstrated by assembling a library of nucleic-acid strands and hairpins as functional modules for evolving networks. Primary T-initiated selection of components from the library assembles a parent CDN X, where the evolved constituents exhibit catalytic properties to cleave the hairpins in the library. Cleavage of the hairpins yields fragments, which reproduces T to replicate CDN X, whereas the other fragments T and T select other components to evolve two other CDNs, Y and Z (variation). By applying appropriate counter triggers, we demonstrate the guided selection of networks from the evolved CDNs. By integrating additional hairpin substrates into the system, CDN-dictated emergent catalytic transformations are accomplished. The study provides pathways to construct evolutionary dynamic networks revealing enhanced gated and cascaded functions.
在广泛的研究努力中,我们引入了基于核酸的构象动态网络(CDN)的进化,这些网络遵循复制/变异/选择原则,以产生高通量的基因进化合成及其功能筛选。这些基本原则通过组装核酸链和发夹作为进化网络的功能模块来证明。从库中选择组件的主要 T 起始选择组装一个父 CDN X,其中进化成分表现出催化特性以切割库中的发夹。发夹的切割产生片段,这些片段通过复制 T 来复制 CDN X,而其他片段 T 和 T 选择其他组件来进化另外两个 CDN,Y 和 Z(变异)。通过应用适当的反触发,我们证明了从进化的 CDN 中进行网络的有指导选择。通过将额外的发夹底物整合到系统中,完成了 CDN 指令的突发催化转化。该研究提供了构建进化动态网络的途径,揭示了增强的门控和级联功能。