Propagation of Enzyme-Induced Surface Events inside Polymer Nanoassemblies for a Fast and Tunable Response


Zhuang J., Secinti H. , Zhao B., Thayumanavan S.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, vol.57, no.24, pp.7111-7115, 2018 (Journal Indexed in SCI) identifier identifier identifier

  • Publication Type: Article / Article
  • Volume: 57 Issue: 24
  • Publication Date: 2018
  • Doi Number: 10.1002/anie.201803029
  • Title of Journal : ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
  • Page Numbers: pp.7111-7115
  • Keywords: electrostatic complexes, enzyme-responsive polymers, host-guest systems, self-assembly, self-immolation, BLOCK-COPOLYMERS, NANOPARTICLES, DELIVERY, PEPTIDES, NANOGELS, RELEASE, PROTEIN, PAYLOAD

Abstract

We report a new molecular design strategy that allows for the propagation of surface enzymatic events inside a supramolecular assembly for accelerated molecular release. The approach addresses a key shortcoming encountered with many of the currently available enzyme-induced disassembly strategies, which rely on the unimer-aggregate equilibria of amphiphilic assemblies. The enzymatic response of the host to predictably tune the kinetics of guest-molecule release can be programmed by controlling substrate accessibility through electrostatic complexation with a complementary polymer. Accelerated guest release in response to the enzyme is shown to be accomplished by a cooperative mechanism of enzyme-triggered supramolecular host disassembly and host reorganization.