Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 38, Pages 21062-21068Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202107917
Keywords
cyclodextrin; enzyme catalysis; hydrogels; non-equilibrium systems; self-regulating behavior
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Funding
- CIM IMPRS Graduate School doctoral fellowship
- Projekt DEAL
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This study demonstrates that hydrogels can be transformed into self-regulating materials by introducing specific substances, resulting in feedback generation in response to external stimuli. The responsive behavior is driven by interactions between specific enzyme-fuel couples, and can be controlled by varying the concentration of added reduction fuel.
Chemical reaction networks (CRN) embedded in hydrogels can transform responsive materials into complex self-regulating materials that generate feedback to counter the effect of external stimuli. This study presents hydrogels containing the beta-cyclodextrin (CD) and ferrocene (Fc) host-guest pair as supramolecular crosslinks where redox-responsive behavior is driven by the enzyme-fuel couples horse radish peroxidase (HRP)-H2O2 and glucose oxidase (GOx)-d-glucose. The hydrogel can be tuned from a responsive to a self-regulating supramolecular system by varying the concentration of added reduction fuel d-glucose. The onset of self-regulating behavior is due to formation of oxidation fuel in the hydrogel by a cofactor intermediate GOx[FADH(2)]. UV/Vis spectroscopy, rheology, and kinetic modeling were employed to understand the emergence of out-of-equilibrium behavior and reveal the programmable negative feedback response of the hydrogel, including the adaptation of its elastic modulus and its potential as a glucose sensor.
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