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

Abstract

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.

Janus Hydrogel with Both Sticky Adhesion and Slippery Antifouling Properties for Strain Sensing

“…Its molecular structure contains multiple catechol groups that can interact with hydrogen bond donors or receptors on the polymer molecular chain. 30,31 These hydrogen bonding interactions can increase the cohesion of the hydrogel and improve the mechanical strength and toughness of the hydrogel. 32,33 The TA coating was also beneficial in improving the antiswelling capacity of the PVA/PSBMA hydrogel, as shown in Figure S10a−d.…”

“…This was attributed to the fact that TA in the Janus hydrogel is a natural polyphenolic compound. Its molecular structure contains multiple catechol groups that can interact with hydrogen bond donors or receptors on the polymer molecular chain. , These hydrogen bonding interactions can increase the cohesion of the hydrogel and improve the mechanical strength and toughness of the hydrogel. , The TA coating was also beneficial in improving the antiswelling capacity of the PVA/PSBMA hydrogel, as shown in Figure S10a–d. This was because the hydrogen bond interaction between TA and PSBMA was stronger than the hydrogen bond interaction with water molecules, making it difficult for the water molecules to enter the hydrogel network.…”

Injectable hydrogels as emerging drug-delivery platforms for tumor therapy

“…As gluconolactone has the ability to gradually release hydrogen ions, this allows for the slow generation of hydrogen bonding interactions. 48 The disintegration conditions of hydrogels formed through hydrogen bonding primarily depend on the hydrogen bonds' interaction with surrounding water molecules, the forces exerted on the crosslinked interconnecting chains, and external loads strong enough to disrupt the crosslinks, and change the network's microstructure, leading to drug release.…”

Natural polyphenol tannin-immobilized composites: rational design and versatile applications

“…Consequently, the hydrogel coating displayed swelling volume stability, ultra-high strength (>10 MPa), and especially excellent oil–water separation efficiency (>99%). 163 In addition, inspired by the intermediate precursor during biomineralization, Tang et al 164 synthesized a series of polyphenol–macromolecule hydrogels. Herein, polyphenol was concentrated on TA, and macromolecules included PVA, SF (silk fibroin), PEG, and PVP were employed.…”