Poly(vinyl Alcohol) (PVA)-Based Hydrogel Scaffold with Isotropic Ultratoughness Enabled by Dynamic Amine–Catechol Interactions

Abstract

Hydrogels, serving as promising load-bearing materials, often suffer from limited long-term stability due to their insufficient mechanical strength. One of the viable methods is to engineer hydrogels with muscle-like anisotropic structures to enable mechanical reinforcement along the alignment direction (e.g., artificial tendons) while sacrificing the mechanical strength in the perpendicular direction. However, for connective tissues such as the fibrous membranes of the articular capsule with fibers interwoven to resist excessive stretching and distension in multiple directions, isotropic mechanical strength is highly demanding. In this work, inspired by the dynamic amine-catechol interactions derived from mussel foot proteins (Mfps), an innovative strategy is developed to incorporate Mfps-like conjugates as elastic connections into the poly­(vinyl alcohol) (PVA) matrix, mimicking the multidirectional fibrous bundles of connective tissues. Superior isotropic tensile strength (13.3 ± 0.5 MPa), ultratoughness (60.1 ± 2.6 MJ/m3), and resilience are achieved in this hydrogel, which surpasses most of the reported biocompatible hydrogels. Additionally, this hydrogel exhibits diverse functionalities such as underwater adhesion and conductivity due to the multiple dynamic amine-catechol interactions engineered in the hydrogel. The versatility of this hydrogel offers a broad range of possibilities as artificial scaffolds with enhanced isotropic mechanical strength and cell affinity for the long service term.

Bio-Inspired Homogeneous Conductive Hydrogel with Flexibility and Adhesiveness for Information Transmission and Sign Language Recognition

“…Except for the high-density hydrogen bonds between adenine and hydrophilic substrates, the metal complexion and π–π stacking also contributed universal adhesion. Hydrophobic substrates with electrostatic charge interacted with the zwitterionic monomer through ion–dipole and dipole–dipole interactions, and the effect also presented on other substrates with polar groups, such as carboxyl groups on skin, amino groups on peptide chains, and hydroxyl groups on woods. , …”

“…Hydrophobic substrates with electrostatic charge interacted with the zwitterionic monomer through ion−dipole and dipole−dipole interactions, and the effect also presented on other substrates with polar groups, such as carboxyl groups on skin, amino groups on peptide chains, and hydroxyl groups on woods. 57,58 3.7. Application of the H-A-CP Hydrogels as Strain Sensor.…”

Kneading-Dough-Inspired Quickly Dispersing of Hydrophobic Particles into Aqueous Solutions for Designing Functional Hydrogels

“…Hydrogels are three-dimensional polymer networks that have received great attention because of their high-water contents and good flexibility [ 1 ]. Composite hydrogels with tunable chemical and physical properties are excellent candidates for bio-medical research [ 2 , 3 ], oil production [ 4 ], adsorbents for removing hazardous pollutants [ 5 , 6 ] underwater adhesive [ 7 ], and other engineering applications [ 8 , 9 ]. Polyethyleneimine (PEI) is a positively charged polymer with a repetition of the ethyleneimine motif in the molecule structure [ 10 ].…”

Doping nanocellulose crystal with poly(vinyl alcohol) for water‐resistant composite fibers with enhanced mechanical and dyeing performances

“…Composite fibers have received widespread attention in recent years due to the high specific strength and performance designability 1,2 . Among them, poly(vinyl alcohol) (PVA)‐based composite fibers offer excellent strength and high modulus, acid and alkali resistance, nontoxic, and wear‐resistant, which makes them one of the most important composite fibers 3–6 . However, untreated PVA fibers with polyhydroxyl structure have very poor water resistance, which limits the usage of PVA fibers in the field of textiles and apparel.…”

“…1,2 Among them, poly(vinyl alcohol) (PVA)-based composite fibers offer excellent strength and high modulus, acid and alkali resistance, nontoxic, and wear-resistant, which makes them one of the most important composite fibers. [3][4][5][6] However, untreated PVA fibers with polyhydroxyl structure have very poor water resistance, which limits the usage of PVA fibers in the field of textiles and apparel. Acetalization with aldehydes is a standard process for increasing the water resistance of PVA fibers, which could additionally enhance the mechanical qualities of PVA fibers.…”