Temporal control of gelation and polymerization fronts driven by an autocatalytic enzyme reaction

Elizabeth Jee, Tamás Bánsági, Annette F. Taylor, John A. Pojman

Research output: Contribution to journalArticlepeer-review

99 Citations (SciVal)

Abstract

Chemical systems that remain kinetically dormant until activated have numerous applications in materials science. Herein we present a method for the control of gelation that exploits an inbuilt switch: the increase in pH after an induction period in the urease-catalyzed hydrolysis of urea was used to trigger the base-catalyzed Michael addition of a water-soluble trithiol to a polyethylene glycol diacrylate. The time to gelation (minutes to hours) was either preset through the initial concentrations or the reaction was initiated locally by a base, thus resulting in polymerization fronts that converted the mixture from a liquid into a gel (ca. 0.1mm min-1). The rate of hydrolytic degradation of the hydrogel depended on the initial concentrations, thus resulting in a gel lifetime of hours to months. In this way, temporal programming of gelation was possible under mild conditions by using the output of an autocatalytic enzyme reaction to drive both the polymerization and subsequent degradation of a hydrogel.

Original languageEnglish
Pages (from-to)2127-2131
Number of pages5
JournalAngewandte Chemie - International Edition
Volume55
Issue number6
Early online date6 Jan 2016
DOIs
Publication statusPublished - 5 Feb 2016

Bibliographical note

Funding Information:
We acknowledge support from the National Science Foundation (CBET 1511653), EPSRC grant EP/K030574/1, and ERC Marie Curie International Incoming Fellowship (PIIF-GA- 2010-274677). We thank Bruno Bock for supplying samples of Thiocure ETTMP 1300. We also thank Dr. Quinlin Wu for use of his rheometer, Kunlin Song for help with using the rheometer, and Dr. Chris Holland for rheometry advice.

Keywords

  • biochemical networks
  • dynamic materials
  • frontal polymerization
  • gels
  • systems chemistry

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Fingerprint

Dive into the research topics of 'Temporal control of gelation and polymerization fronts driven by an autocatalytic enzyme reaction'. Together they form a unique fingerprint.

Cite this