葡萄糖氧化酶
超分子化学
自愈水凝胶
化学
酶
氧化还原
二茂铁
组合化学
化学工程
电化学
高分子化学
有机化学
电极
分子
物理化学
工程类
作者
Mehak Jain,Bart Jan Ravoo
标识
DOI:10.1002/anie.202107917
摘要
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 β-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)-H2 O2 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[FADH2 ]. 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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