Biomineralization-Inspired Intermediate Precursor for the Controllable Gelation of Polyphenol–Macromolecule Hydrogels

Hydrogels composed of polyphenols and various macromolecules have been widely reported to have the advantage of facile preparation, mainly through the formation of hydrogen bonds. However, the traditional preparation method involves the direct mixing of polyphenols and macromolecules, which generally occurs too quickly and uncontrollably, and results in poor homogeneity, injectability, and shape designability. Here, inspired by the intermediate precursor during biomineralization, to facilitate transformation in a controllable way, we propose a novel and universal internal gelation method that creates an intermediate precursor by controlling the pH value to manipulate the elimination and generation of hydrogen bonds between a polyphenol and macromolecules. The precursor strategy greatly improves the homogeneity, injectability, and shape designability of the hydrogel while also achieving a controllable gelation process, and the gelation time can be accurately adjusted. The hydrogels prepared with this method exhibited superior capability to seal leaks, provided complete wound coverage, and showed the potential to be a shape-designable wearable strain sensor. Our study opens up a new way to construct and apply polyphenol-macromolecule hydrogels in a more controllable manner.