Self-Sorting in Dynamic Combinatorial Libraries Leads to the Co-Existence of Foldamers and Self-Replicators.
Self-Sorting in Dynamic Combinatorial Libraries Leads to the Co-Existence of Foldamers and Self-Replicators.
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DOI：
10.1002/anie.202101052
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发表时间：
2021-06-07
期刊：
影响因子：
--
通讯作者：
Otto S
中科院分区：
文献类型：
--
作者：
Liu B;Beatty MA;Pappas CG;Liu K;Ottelé J;Otto S
自然界在两种不同的化合物类别（例如用于复制的多核苷酸和用于催化的折叠聚酰胺）之间分离了信息存储/传输和催化等基本任务。这种分工很可能是进化的产物，这就提出了一个问题：在从化学到生物学的过渡中，复制因子和折叠大分子共存的更简单的系统是如何出现的？在合成系统中，实现复制子和文件夹在单个分子网络中共存仍然是一个未解决的问题。先前对动态分子网络的研究已经产生了自我复制的纤维或定义良好的文件夹结构（或完全未分类的复杂系统）。我们报告了一个系统，其中两个交叉反应的二硫醇（核碱基和肽基）构建块自分类成一个复制子纤维和文件夹，两者自发出现并共存。自分类行为在不同的构建块比例中仍然普遍存在，因为出现了两个阶段：复制子生长和文件夹形成。这归因于复制子纤维的自催化形成，随后在剩余的构建块中富集系统，随后将其纳入文件夹。两个不同的二硫醇构建块通过可逆共价键相互转换，最初形成各种大小的动态组合库。自分类过程从单个库成员的扩增开始，形成自我复制的纤维。这一步之后是在剩余的构建块中富集系统，形成一个大的大环文件夹。
Nature segregates fundamental tasks such as information storage/transmission and catalysis between two different compound classes (e.g. polynucleotides for replication and folded polyamides for catalysis). This division of labor is likely a product of evolution, raising the question of how simpler systems in which replicators and folded macromolecules co‐exist may emerge in the transition from chemistry to biology. In synthetic systems, achieving co‐existence of replicators and foldamers in a single molecular network remains an unsolved problem. Previous work on dynamic molecular networks has given rise to either self‐replicating fibers or well‐defined foldamer structures (or completely un‐sorted complex systems). We report a system in which two cross‐reactive dithiol (nucleobase‐ and peptide‐based) building blocks self‐sort into a replicator fiber and foldamer that both emerge spontaneously and co‐exist. The self‐sorting behavior remains prevalent across different building block ratios as two phases of emergence occur: replicator growth followed by foldamer formation. This is attributed to the autocatalytic formation of the replicator fiber, followed by enrichment of the system in the remaining building block, which is subsequently incorporated into a foldamer. Two different dithiol building blocks interconvert through reversible covalent bonds to initially form a dynamic combinatorial library of macrocycles of various size. The self‐sorting process starts by the amplification of a single library member to form self‐replicating fibers. This step is followed by enrichment of the system in the remaining building block, which forms a large macrocyclic foldamer.
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