Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem, 91904, Israel.
Angew Chem Int Ed Engl. 2019 Aug 26;58(35):12238-12245. doi: 10.1002/anie.201905235. Epub 2019 Jul 26.
The evolution of networks is a fundamental unresolved issue in developing the area of systems chemistry. We introduce a versatile rewiring mechanism that leads to the emergence of nucleic-acid-based constitutional dynamic networks (CDNs). A two-component constituent AA' functionalized with a Mg -ion-dependent DNAzyme activator unit forms a complex with an intact hairpin H composed of B and B' sequences. Cleavage of H leads to the two-component constituent BB', and its rewiring with AA' yields CDN X composed of the equilibrated constituents AA', AB', BA', and BB'. In analogy, subjecting AA' to an intact hairpin H leads to the formation of CDN Y consisting of AA', AC', CA', and CC'. Subjecting AA' to the mixture of H and H evolves the [3×3] CDN Z, composed of nine constituents, thus demonstrating hierarchical adaptive properties. Furthermore, the DNAzyme units associated with the constituents are applied to tailor emerging catalytic functions from the different CDNs.
网络的演化是系统化学领域发展中一个未解决的基本问题。我们引入了一种通用的重连机制，该机制导致基于核酸的结构动态网络（CDN）的出现。由与 Mg 离子依赖性 DNA 酶激活单元功能化的两个组件 AA'与由 B 和 B'序列组成的完整发夹 H 形成复合物。H 的切割导致两个组件 BB'，其与 AA'的重连生成由平衡的组件 AA'、AB'、BA'和 BB'组成的 CDN X。类似地，使 AA'经受完整的发夹 H 导致由 AA'、AC'、CA'和 CC'组成的 CDN Y 的形成。使 AA'经受 H 和 H 的混合物可进化出由九个组成部分组成的[3×3]CDN Z，从而展示了分层自适应特性。此外，与组成部分相关联的 DNA 酶单元被应用于从不同的 CDN 中定制新兴的催化功能。
