Polysaccharide-Based Injectable Hydrogels with Fast Gelation and Self-Strengthening Mechanical Kinetics for Oral Tissue Regeneration.

Oral defects lead to a series of function disorders, severely threatening the patients' health. Although injectable hydrogels are widely studied in tissue regeneration, their mechanical performance is usually stationary after implant, without further self-adaption toward the microenvironment. Herein, an injectable hydrogel with programmed mechanical kinetics of instant gelation and gradual self-strengthening along with outstanding biodegradation ability is developed. The fast gelation is realized through rapid Schiff base reaction between biodegradable chitosan and aldehyde-modified sodium hyaluronate, while self-strengthening is achieved via slow reaction between redundant amino groups on chitosan and epoxy-modified hydroxyapatite. The resultant hydrogel also possesses multiple functions including (1) bio-adhesion, (2) self-healing, (3) bactericidal, (4) hemostasis, and (5) X-ray in situ imaging, which can be effectively used for oral jaw repair. We believe that the strategy illustrated here will provide new insights into dynamic mechanical regulation of injectable hydrogels and promote their application in tissue regeneration.

Photo-switchable supramolecular comb-like polymer brush based on host-guest recognition for use as antimicrobial smart surface.

Bacterial infections from biomedical devices pose a great threat to the health of humans and thus place a heavy burden on society. Therefore, developing efficient antibacterial surfaces has attracted much attention. However, it is a challenge to identify or develop a combination that efficiently integrates multiple functions via topological tailoring and on-demand function-switch via non-contact and noninvasive stimuli. To resolve this issue, a highly hydrophilic comb polymer brush was constructed here based on supramolecular host-guest recognition. Azobenzene (azo)-modified antifouling and antibacterial polymers were incorporated into cyclodextrin (CD)-modified antifouling polymer brushes grafted on the surface. The surface thus obtained possessed excellent antifouling performance with a low bacterial density of ∼6.25 × 105 cells per cm2 after 48 h and exhibited a high efficiency of ∼88.2% for killing bacteria. Besides, irradiation with UV light resulted in the desorption of the azo-polymers and a release of ∼85.1% attached bacteria. Irradiating visible light led to the re-adsorption of azo-polymers, which regenerated the fresh surface; the process could be repeated for at least three cycles, and the surface still maintained low bacterial attachments with a cell density of ∼7.10 × 105 cells per cm2, high sterilization efficiency of ∼93.8%, and a bacteria release rate of ∼83.1% in the 3rd cycle. The photo-switchable antibacterial surface presented in this research will provide new insights into the development of smart biomedical surfaces.

Cationic peptide-based salt-responsive antibacterial hydrogel dressings for wound healing.

Development of biological dressings has received widespread attentions due to their good breathability, biocompatibility, wettability, and the ability to absorb wound exudate without sticking to the wound. However, current proposed antibacterial hydrogels are limited antibacterial ability, short service life and insufficient biocompatibility, which are still challenging to address intricate practical applications. Here we develop a cationic peptide-based, salt-responsive hydrogel dressing with triple functions of antifouling, bactericidal, and bacterial release by combining ε-poly-l-lysine, poly(ethylene glycol) diglycidyl ether, and poly(DVBAPS-co-GMA) via a one-pot method. These designed hydrogels enabled to further quaternize to enhance antibacterial property due to the presence of amine residues. The resultant hydrogels present good antibacterial activity (>90%), biocompatibility, cell proliferation efficacy (~400%) and adhesiveness. Through in vivo and in vitro antibacterial capability tests, it is also found that hydrogels have good antifouling and sterilization capabilities, and the sterilization rate could reach up to ~96%. In addition, ~94% of the attached bacterial can be released after saline/water switching for several cycles. Taken together, the designed multiple antibacterial dressing prolongs the lifespan relying on reversible salt-responsive release and meet special requirements for wound healing. This work not only provides a platform to highlight its promising potentials in wound management but also gives a custom strategy to biomedical applications.

Programmable Deformations of Biomimetic Composite Hydrogels Embedded with Printed Fibers.

Shape deformations are prevalent in nature, which are closely related to the heterogeneous structures with a feature of fibrous elements embedded in a matrix. The microfibers with specific orientations act as either passive geometrical constraints in an active matrix or active elements in a passive matrix, which generate programmed internal stresses and drive shape morphing under external stimuli. Morphing materials can be designed in a biomimetic way, yet it is challenging to fabricate composite hydrogels with well-distributed fibers by a facile strategy. Here, we demonstrate the fabrication of microfiber-embedded hydrogels facilitated by the extrusion-based printing technology. Programmed deformations are achieved in these hydrogels with microfibers distributed in the upper and/or bottom layers of the gel matrix. Under external stimuli, the microfibers and the gel matrix have different responses that produce internal stresses and result in programmable deformations of the composite gel. Multiple shape transformations are realized in the hydrogel by embedding multiple types of responsive microfibers in the passive or active matrix, which is fabricated with the assistance of multinozzle printing. A soft hook is designed to show the capacity of the composite hydrogel to hold and move an object in a saline solution. This facile and versatile strategy provides an alternative way to prepare biomimetic hydrogels with potential applications in biomedical devices, flexible electronics, and soft robots.