期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 6, 页码 2127-2131出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201510604
关键词
biochemical networks; dynamic materials; frontal polymerization; gels; systems chemistry
资金
- National Science Foundation [CBET 1511653]
- EPSRC [EP/K030574/1]
- ERC Marie Curie International Incoming Fellowship [PIIF-GA-2010-274677]
- Engineering and Physical Sciences Research Council [EP/K030574/2, EP/K030574/1] Funding Source: researchfish
- EPSRC [EP/K030574/2, EP/K030574/1] Funding Source: UKRI
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. 0.1mmmin(-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.
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