Multifunctional self-healing hydrogels have recently attracted considerable interest in biomedical applications owing to their diverse properties, including self-healing, adhesion, conduction, antibacterial, and stimulus-response, which can meet various application requirements, ranging from wound dressings and delivery vehicles to the production of scaffolds for tissue repair and regeneration. As a natural polycationic polysaccharide with good biocompatibility, chitosan is widely used in hydrogel formation as there are many amino and hydroxyl groups along the chains that can actively participate in various physical effects and chemical reactions, which enable it to construct self-healing hydrogels and fulfill multiple functions. In this review, the formation of chitosan-based self-healing hydrogels and the related self-healing mechanism are summarized, including Schiff base, metal coordination, ionic and hydrogen bonds, hydrophobic and host-guest interactions, with a focus on the strategies for their multi-functionalization. In the last section, the applications of the chitosan-based self-healing hydrogels in the fields of wound dressings, delivery vehicles, scaffolds, and biological sensors are discussed. Overall, it is highly expected that this review could provide an insight into the prospective development of multifunctional self-healing hydrogels for biomedical applications.

Advances in multifunctional chitosan-based self-healing hydrogels for biomedical applications.

Preparation of a Strong, Mildew-Resistant, and Flame-Retardant Biomimetic Multifunctional Soy Protein Adhesive Via the Construction of an Organic-Inorganic Hybrid Multiple-Bonding Structure

Preparation of a strong, mildew-resistant, and flame-retardant biomimetic multifunctional soy protein adhesive via the construction of an organic-inorganic hybrid multiple-bonding structure

rGO/MXene sandwich-structured film at spunlace non-woven fabric substrate: Application to EMI shielding and electrical heating.

Spider silk-inspired high-performance soybean meal-based adhesive reinforced by greenly produced chitosan-functionalized boron nitride nanosheets

Soy protein (SP)-based adhesives can replace traditional aldehyde-based adhesives for the manufacturing of wood-based panels. However, developing a SP-based adhesive with excellent prepressing bonding strength, flame retardancy, and mildew resistance remains a challenge. Herein, an inorganic crystal cross-linked hybrid SP adhesive was developed inspired by the "secreting-hardening" process of the mussel adhesive protein and the organic-inorganic hybrid adhesive system of the oyster. Calcium sulfoaluminate (CSA) was introduced into the adhesive mixture of SP and acrylic acid to induce the in situ polymerization of acrylic acid to achieve adhesive gelation. The generation of the inorganic crystals by hydration of CSA not only contributed to the formation of a stable cross-linked hybrid adhesive system for strong cohesion but also provided strong interfacial adhesion between the adhesive layers and the plywood veneers. As anticipated, the prepared plywood sample bonded with the hybrid adhesive gel had an excellent prepressing bonding strength of 544 kPa, representing a significant increase compared to that of the pure SP adhesive (19 kPa). Moreover, the generated inorganic crystals endowed the adhesive with excellent mildew resistance and flame retardancy. This study provides a novel and effective strategy for the preparation of high-performance SP-based adhesives.

Novel Bionic Soy Protein-Based Adhesive with Excellent Prepressing Adhesion, Flame Retardancy, and Mildew Resistance.

Multifunctional hydrogels that integrate stretchability, adhesion, self-healing, and antibacterial properties may find use in a variety of fields including electronic skin, wound dressings, and wearable devices; however, traditional hydrogels often exhibit short-term adhesiveness, poor mechanical properties, and a lack of antibacterial activity. Herein, a plant-inspired polyacrylamide-soybean protein isolate-pyrogallol/borax (PAM-SPI-P/B) hydrogel has been developed using a facile green method based on dynamic coordination cross-linking between pyrogallol (PG) and borax. The PG–borax dynamic bonds adjusted the network structure of the hydrogels to provide greater structural integrity to the PAM–SPI double network. This hydrogel possessed a high mechanical strength (large elongation up to 760% and compressive strength up to 1.25 MPa at 80% strain), low swelling ratio, and self-healing properties. Inspired by natural polyphenols that contain adhesive molecules, the addition of pyrogallol provided the hydrogel excellent adhesion to various hydrophilic and hydrophobic substrates. And with the inhibition of pyrogallol autoxidation due to the borax protection, the hydrogel showed repeatable and durable adhesion over 20 cycles. The obtained hydrogels also exhibited good antibacterial activities against Escherichia coli and Staphylococcus aureus because they were based on pyrogallol and borax, which have antibacterial properties. Accordingly, we envision that the PAM-SPI-P/B hydrogels have great potential for use in biomimetic tissues and biosensors.

A tough, adhesive, self-healable, and antibacterial plant-inspired hydrogel based on pyrogallol-borax dynamic cross-linking.

Although humidity-responsive actuators serve as a promising candidate in smart wearables, artificial muscles, and biomimetic devices, most of them derived from synthetic polymers could not simultaneously achieve multifunctional properties. In this work, a cellulose nanofiber (CNF)-based film actuator with high mechanical properties, excellent Joule heating, and antibacterial capability is successfully constructed by integrating with Ti3C2Tx (MXene) and tannic acid (TA) via a vacuum-assisted filtration approach. Owing to the unique nacrelike structure and strong hydrogen bonds, the tensile strength and toughness of the composite film could reach 275.4 MPa and 10.2 MJ·m-3, respectively. Importantly, the hydrophilic nature of CNFs and alterable interlayer spacing of MXene nanosheets endow the composite film with sensitive humidity response and extraordinary stability (1000 cycles). With the assistance of MXene nanosheets and TA, the composite film could not only present outstanding Joule heating but also possess remarkable antibacterial properties against both Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus. Benefiting from the above merits, the proof-of-concept smart garment is assembled by the as-prepared film and is capable of regulating humidity and temperature.

Chao Ma

Papers

Novel Bionic Soy Protein-Based Adhesive with Excellent Prepressing Adhesion, Flame Retardancy, and Mildew Resistance.

A tough, adhesive, self-healable, and antibacterial plant-inspired hydrogel based on pyrogallol-borax dynamic cross-linking.

Tough and Multifunctional Composite Film Actuators Based on Cellulose Nanofibers toward Smart Wearables.

Plant Polyphenol-Inspired Crosslinking Strategy toward High Bonding Strength and Mildew Resistance for Soy Protein Adhesives

Facile strategy of mussel-inspired polymer as a high-performance dry/wet adhesive