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Non-enzymatic bistable chemical networks. Angew. Chem. 2015; Nature Commun. 2019


Remarkable developments in Systems Chemistry over the past decade offer alternative strategies for the bottom-up design of entirely synthetic molecular networks with life-like functions. Most significantly, recent progress has been achieved via the development of schemes for operating out of equilibrium, which have so far  provided access to transient structures that form as a result of constant energy dissipation. We have shown that the study of chemical networks out of equilibrium further allow control over dynamical network-dependent functions. We have exploited thiodepsipeptide-based non-enzymatic networks propelled by reversible replication processes out of equilibrium, presenting bistable behaviour. Bistability was reached due to a disparity between forward and backward processes and is accessible only as long as energy is supplied by a reducing agent. Using theory, simulation ​and experiments, we characterized the bistable behaviour of the networks under a wide range of conditions and established the limits and req​uirements for phase transitions from 'ordinary' behaviour – leading to a single steady state – to bistable functionality. We envision that the development of biomimetic bistable systems will pave the way to the study of more elaborate functions in synthetic networks, such as information transfer and signalling.

 

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