CHAPTER 4: Enzyme-Responsive Molecular Gels

This chapter details recent developments in the use of biocatalytic reactions to control and direct supramolecular gelation of peptide derivatives. The use of biocatalysis in this context provides a powerful approach for the development of ‘smart’ biomaterials in that it combines biological selectivity and catalytic amplification with the versatility of the bottom-up nanofabrication through dynamic self-assembly. The design rules of the self-assembly building blocks and biocatalytic switch components are discussed. Then, we will discuss a number of unique features of these systems, including the possibility of controlling mechanical properties, construction of variable structures from identical chemical components exploiting kinetically controlled systems and the defect correcting and component-selecting capabilities of the systems that operate under thermodynamic control. Applications of these biocatalytic gels are discussed in context of (intracellular) biosensing, controlled release and cell instructive materials that control and direct cell fate.