Enzyme Assisted Self-Assembly (EASy)

Self-assembly (SA) as an approach to produce functional molecular architectures is commonplace in biology. Despite significant advances it is still a major challenge to achieve similar control and complexity in the laboratory. We have discovered the use of fully reversible enzyme catalysed reactions to drive SA. In this approach, molecular self-assembly provides a thermodynamic driving force that enables a protease to produce building blocks in a reversible and spatially confined manner. We demonstrate that this system uniquely combines three features: (i) self-correction: fully reversible SA under thermodynamic control, (ii) component-selection: the ability to amplify the most stable molecular SA structures in dynamic combinatorial libraries, (iii) spatiotemporal confinement of nucleation and structure growth. Enzyme-assisted SA therefore provides unprecedented control in bottom-up fabrication of nanomaterials, ultimately paving the way to functional nanostructures with enhanced complexities and fewer defects.

[1] R.J. Williams, A.M. Smith, R. Collins, N. Hodson, A.K. Das, R.V. Ulijn, Enzyme Assisted Self-Assembly under Thermodynamic Control, Nature Nanotechnology, 2009, 4, 19-24.
[2] S. Toledano, R.J. Williams, V. Jayawarna, R.V. Ulijn. Enzyme triggered self-assembly of peptide hydrogels via reversed hydrolysis. J. Am. Chem. Soc., 2006, 128, 1070-1071.