College of Life Science and Technology, Beijing University of Chemical Technology, Beijing 100029, People's Republic of China.
ACS Nano. 2022 Sep 27;16(9):14274-14283. doi: 10.1021/acsnano.2c04405. Epub 2022 Sep 14.
Live cells precisely control their temporal pattern in energy dissipative processes such as catalysis and assembly. Here, we demonstrate a DNA-based artificial dissipative nonequilibrium system where the transient state is controlled by the processive digestion of λ-exonuclease (λ Exo). This enzyme reaction serves as an orthogonal and independent molecular timer allowing for the programmable regulation of the transient-state lifetime. This dissipation system is concatenated to enzyme catalysis and nanostructure assembly networks. Dynamic activation of enzyme catalysis and dynamic disassembly of DNA nanotubes (DNT) are realized, and the state lifetimes of these systems are accurately encoded by the DNA timer. This work demonstrates nontrivial dissipation systems with built-in molecular timers, which can be a useful tool for developing artificial reaction networks and nanostructures with enhanced complexities and intelligence.
活细胞在能量耗散过程(如催化和组装)中精确地控制其时间模式。在这里,我们展示了一个基于 DNA 的人工耗散非平衡系统,其中瞬态由 λ-核酸外切酶(λ Exo)的连续消化控制。这种酶反应作为正交且独立的分子定时器,允许对瞬态寿命进行可编程调节。这个耗散系统与酶催化和纳米结构组装网络串联。实现了酶催化的动态激活和 DNA 纳米管(DNT)的动态拆卸,并且这些系统的状态寿命由 DNA 定时器精确编码。这项工作展示了具有内置分子定时器的非平凡耗散系统,这可能是开发具有增强复杂性和智能的人工反应网络和纳米结构的有用工具。