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Biocatalytic reversible control of the stiffness of DNA-modified responsive hydrogels: applications in shape-memory,self-healing and autonomous controlled release of insulin
Authors:Chen Wang  Amit Fischer  Avner Ehrlich  Yaakov Nahmias  Itamar Willner
Affiliation:Institute of Chemistry, The Minerva Center for Bio-hybrid Complex Systems, The Hebrew University of Jerusalem, Jerusalem 91904 Israel.; Grass Center for Bioengineering, Benin School of Computer Science and Engineering, The Hebrew University of Jerusalem, 91904 Israel
Abstract:The enzymes glucose oxidase (GOx), acetylcholine esterase (AchE) and urease that drive biocatalytic transformations to alter pH, are integrated into pH-responsive DNA-based hydrogels. A two-enzyme-loaded hydrogel composed of GOx/urease or AchE/urease and a three-enzyme-loaded hydrogel composed of GOx/AchE/urease are presented. The biocatalytic transformations within the hydrogels lead to the dictated reconfiguration of nucleic acid bridges and the switchable control over the stiffness of the respective hydrogels. The switchable stiffness features are used to develop biocatalytically guided shape-memory and self-healing matrices. In addition, loading of GOx/insulin in a pH-responsive DNA-based hydrogel yields a glucose-triggered matrix for the controlled release of insulin, acting as an artificial pancreas. The release of insulin is controlled by the concentrations of glucose, hence, the biocatalytic insulin-loaded hydrogel provides an interesting sense-and-treat carrier for controlling diabetes.

Biocatalytic control over the stiffness of pH-responsive hydrogels is applied to develop shape-memory, self-healing and controlled release matrices.
Keywords:
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