Volume 54, Issue 45 pp. 13258-13262
Communication

Biocatalytic Feedback-Driven Temporal Programming of Self-Regulating Peptide Hydrogels

Thomas Heuser

Thomas Heuser

DWI—Leibniz Institute for Interactive Materials, Forckenbeckstrasse 50, 52056 Aachen (Germany) http://www.dwi.rwth-aachen.de

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Elisabeth Weyandt

Elisabeth Weyandt

DWI—Leibniz Institute for Interactive Materials, Forckenbeckstrasse 50, 52056 Aachen (Germany) http://www.dwi.rwth-aachen.de

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Dr. Andreas Walther

Corresponding Author

Dr. Andreas Walther

DWI—Leibniz Institute for Interactive Materials, Forckenbeckstrasse 50, 52056 Aachen (Germany) http://www.dwi.rwth-aachen.de

DWI—Leibniz Institute for Interactive Materials, Forckenbeckstrasse 50, 52056 Aachen (Germany) http://www.dwi.rwth-aachen.deSearch for more papers by this author
First published: 06 August 2015
Citations: 243

Graphical Abstract

Programmed to self-destruct: An internal enzymatic feedback system enables the autonomous self-regulation over time of a pH-responsive peptide gelator (see picture; SA=self-assembly). The resulting dynamic hydrogels with programmed lifetimes are suitable for application in fluidic guidance, burst release, and transient rapid prototyping.

Abstract

Switchable self-assemblies respond to external stimuli with a transition between near-equilibrium states. Although being a key to present-day advanced materials, these systems respond rather passively, and do not display autonomous dynamics. For autonomous behavior, approaches must be found to orchestrate the time domain of self-assemblies, which would lead to new generations of dynamic and self-regulating materials. Herein, we demonstrate catalytic control of the time domain of pH-responsive peptide hydrogelators in a closed system. We program transient acidic pH states by combining a fast acidic activator with the slow, enzymatic, feedback-driven generation of a base (dormant deactivator). This transient state can be programmed over orders of magnitude in time. It is coupled to dipeptides to create autonomously self-regulating, dynamic gels with programmed lifetimes, which are used for fluidic guidance, burst release, and self-erasing rapid prototyping.

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