Department of Chemistry, Ben-Gurion University of the Negev, 84105, Beer Sheva, Israel.
Institute for Macromolecular Chemistry, Albert Ludwigs University of Freiburg, D-79104, Freiburg, Germany.
Nat Commun. 2019 Oct 11;10(1):4636. doi: 10.1038/s41467-019-12645-0.
One of the grand challenges in contemporary systems chemistry research is to mimic life-like functions using simple synthetic molecular networks. This is particularly true for systems that are out of chemical equilibrium and show complex dynamic behaviour, such as multi-stability, oscillations and chaos. We report here on thiodepsipeptide-based non-enzymatic networks propelled by reversible replication processes out of equilibrium, displaying bistability. Accordingly, we present quantitative analyses of the bistable behaviour, featuring a phase transition from the simple equilibration processes taking place in reversible dynamic chemistry into the bistable region. This behaviour is observed only when the system is continuously fueled by a reducing agent that keeps it far from equilibrium, and only when operating within a specifically defined parameter space. We propose that the development of biomimetic bistable systems will pave the way towards the study of more elaborate functions, such as information transfer and signalling.
当代系统化学研究的一大挑战是使用简单的合成分子网络模拟类似生命的功能。对于处于化学平衡之外并表现出复杂动态行为的系统,如多稳定性、振荡和混沌,尤其如此。我们在这里报告了基于硫代二肽的非酶网络,这些网络由远离平衡的可逆复制过程推动,显示出双稳定性。因此,我们对双稳态行为进行了定量分析,其特征是从发生在可逆动态化学中的简单平衡过程到双稳态区域的相变。只有当系统连续受到还原剂的供给时,才会出现这种行为,还原剂使系统远离平衡,并且只有在特定定义的参数空间内运行时才会出现这种行为。我们提出,仿生双稳系统的发展将为研究更复杂的功能铺平道路,如信息传递和信号转导。