A3BMS Lab, Institute for Macromolecular Chemistry , University of Freiburg , Stefan-Meier-Straße 31 , 79104 Freiburg , Germany.
DFG Cluster of Excellence "Living, Adaptive and Energy-Autonomous Materials Systems" (livMatS) , 79110 Freiburg , Germany.
J Am Chem Soc. 2020 Jan 15;142(2):685-689. doi: 10.1021/jacs.9b11598. Epub 2020 Jan 7.
We introduce pathway complexity on a multicomponent systems level in chemically fueled transient DNA polymerization systems, achieving autonomous evolution over multiple structural dynamic steady states from monomers to dimers, oligomers of dimers, and randomized polymer structures before being ultimately degraded back to monomers once the fuel is consumed. The enabling key principle is to design monomer species having kinetically selected molecular recognition in the structure-forming step and which are reconfigured in an enzymatic reaction network. This nonequilibrium systems chemistry approach to pathway complexity provides new conceptual insights into fuel-driven automatons and autonomous materials design.
我们在化学燃料瞬态 DNA 聚合系统中引入了多组分系统级的途径复杂性，实现了从单体到二聚体、二聚体低聚物和随机聚合物结构的自主进化，然后在燃料消耗后最终降解回单体。使能的关键原理是设计具有结构形成步骤中动力学选择分子识别的单体物种，并在酶反应网络中重新配置。这种非平衡系统化学方法途径复杂性为燃料驱动自动机和自主材料设计提供了新的概念见解。
