Repurposing a Catalytic Cycle for Transient Self-Assembly.

Abstract

Life operates out of equilibrium to enable various sophisticated behaviors. Synthetic chemists have strived to mimic biological nonequilibrium systems in such fields as autonomous molecular machines and dissipative self-assembly. Central to these efforts has been the development of new chemical reaction cycles, which drive systems out of equilibrium by conversion of chemical fuel into waste species. However, the construction of reaction cycles has been challenging due to the difficulty of finding compatible reactions that constitute a cycle. Here, we realize an alternative approach by repurposing a known catalytic cycle as a chemical reaction cycle for driving dissipative self-assembly. This approach can overcome the compatibility problem because all steps involved in a catalytic cycle are already known to proceed concurrently under the same conditions. Our repurposing approach is applicable to diverse combinations of catalytic cycles and systems to drive out of equilibrium, which will substantially broaden the scope of out-of-equilibrium systems.