A Minimalistic Covalent Bond-Forming Chemical Reaction Cycle that Consumes Adenosine Diphosphate.

Abstract

The development of active matter requires the ability to design materials capable of harnessing energy from a source to carry out work. Nature achieves this using chemical reaction cycles in which energy released from an exergonic chemical reaction is used to drive biochemical processes. Although many chemically fuelled synthetic reaction cycleshave been reported, the generally high complexity of the reported systems hampers a full understanding of how the available chemical energy is actually exploited by these systems. This lack of understanding is a limiting factor in the design of active matter. Here, we report a minimalistic reaction cycle in which adenosine diphosphate (ADP) triggers the formation of a catalyst for its own hydrolysis. This establishes an interdependence between the concentrations of the network components resulting in the transient formation of the catalyst. The network is sufficiently simple that all kinetic and thermodynamic parameters governing its behaviour can be characterised, allowing kinetic models to be built that simulate the progress of reactions within the network. While the current network does not enable the ADP-hydrolysis reaction to populate a nonequilibrium composition, these models provide insight into the way the network dissipates energy. Furthermore, design principles are revealed for constructing driven systems.