Bioinspired Fuel-driven Living and Transient Supramolecular Polymerization

Recently, we developed a common synthetic strategy that works on biological principles such as chemical fuel-driven control over structural and temporal self-assembly profile. We employ simple yet powerful dynamic covalent bond chemistry, where covalent bonds are being made and broken by synthetic means only, to kinetically control the formation of supramolecular polymer. Here, we apply chemical reaction(s) to activate building blocks to trigger their assembly in a kinetically controlled manner, later returning back to the original state under the same reaction conditions. In our recent work we explored the pH responsive imine chemistry where the design involves the conversion of non-assembling CT complex (inactive/dormant state) between aromatic donor and benzaldehyde substituted viologen acceptor into a self-assembling CT amphiphile (active state) via an in situ kinetically controlled imine bond formation with an alkyl amine (fuel) similar to inactive and active states of protein monomers in biological assemblies which can be triggered by a fuel. Further, in our biomimetic approach, we deployed two orthogonal enzymatic reaction networks to create adaptive, autonomous, and like-life out-of-equilibrium supramolecular materials. 

ATP-fuelled, enzymatically Controlled Approach