Facile Bond Exchanging Strategy for Engineering Wet Adhesion and Antioxidant/Antibacterial Thin Layer over a Dynamic Hydrogel via the Carbon Dots Derived from Tannic Acid/ε-Polylysine.

Adhesive hydrogels, playing an essential role in stretchable electronics, soft robotics, tissue engineering, and so forth, upon functioning often need to adhere to various substrates in wet conditions and simultaneously exhibit antibacterial/antioxidant properties while possessing the intrinsic stretchability and elasticity of the hydrogel network intact. Therefore, simple approaches to conveniently access adhesive hydrogels with multifunctional surfaces are being pursued. Herein, a facile strategy has been proposed to construct multifunctional adhesive hydrogels via surface engineering of a multifunctional carbon dot (CD)-decorated polymeric thin layer by dynamic bond exchange. By this strategy, a double cross-linked network hydrogel of polyacrylamide (PAM) and oxidized dextran (ODA) was engineered with a unique dense layer over the Schiff base hydrogel matrix by aqueous solution immersion of PA-120, versatile CDs derived from tannic acid (TA) and ε-polylysine (PL). Without any additional agents, the PA-120 CDs with residual polyphenolic/catechol and amine moieties were incorporated into the surface structure of the hydrogel network by the combined action of the Schiff base and hydrogen bonds to form a dense surface layer that can exhibit high wet adhesive performance via the amine-polyphenol/catechol pair. The armor-like dense architecture also endowed hydrogels with considerably enhanced tensile/compression properties and excellent antioxidant/antibacterial abilities. Besides, the single-sided modified Janus hydrogel and completely surface-modified hydrogel can be flexibly developed through this approach. This strategy will provide new insights into the preparation and application of surface-modified hydrogels featuring multiple functions and tunable interfacial properties.

Recent Progress on Chiral Carbon Dots: Synthetic Strategies and Biomedical Applications.

The discovery of chiral carbon dots (Ch-CDs) has opened up an exciting new research direction in the field of carbon dots. It not only retains the chirality of the precursor and exhibits highly symmetric chiral optical properties but also has properties such as chemical stability, antibacterial and antitumor properties, and good biocompatibility of carbon dots. Based on these advantages, the application of Ch-CDs in the biomedical field has attracted significant interest among researchers. However, a comprehensive review of the selection of precursors for Ch-CDs, preparation methods, and applications in biomedical fields is still lacking. Here, we summarize their precursor selection and preparation methods based on recent reports on Ch-CDs and provide the first comprehensive review for specific applications in biomedical engineering, such as biosensing, bioimaging, drug carriers, antibacterial and antibiofilm, and enzyme activity modulation. Finally, we discuss application prospects and challenges that need to be overcome. We hope this review will provide valuable guidance for researchers to prepare novel Ch-CDs and facilitate their application in biomedical engineering.

Transformation of arginine into zero-dimensional nanomaterial endows the material with antibacterial and osteoinductive activity.

Implant-associated infection is a major threat affecting the success of orthopedic surgeries. Although various materials scavenge bacteria by generating reactive oxygen species (ROS), the intrinsic inability of ROS to distinguish bacteria from cells notably limits the therapeutic effects. Here, we found that the arginine carbon dots (Arg-CDs) that were transformed from arginine exhibited supreme antibacterial and osteoinductive activity. We further designed the Schiff base bond between Arg-CDs and aldehyde hyaluronic acid/gelatin methacryloyl (HG) hydrogel to release Arg-CDs in response to the acidic bone injury microenvironment. The free Arg-CDs could selectively kill bacteria by generating excessive ROS. Furthermore, the Arg-CD-loaded HG composite hydrogel showed excellent osteoinductive activity through inducing the M2 polarization of macrophages by up-regulating interleukin-10 (Il10) expression. Together, our findings revealed that transformation of the arginine into zero-dimensional Arg-CDs could endow the material with exceptional antibacterial and osteoinductive activity, favoring the regeneration of infectious bone.

Antibacterial and antibiofilm mechanisms of carbon dots: a review.

Due to the increasing bacterial resistance to conventional antibiotics, developing safe and effective approaches to combat infections caused by bacteria and biofilms has become an urgent clinical problem. Recently, carbon dots (CDs) have received great attention as a promising alternative to conventional antimicrobial agents due to their excellent antimicrobial efficacy and biocompatibility. Although CDs have been widely used in the field of antibacterial applications, their antibacterial and antibiofilm mechanisms have not been systematically discussed. This review provides a systematic overview on the complicated mechanisms of antibacterial and antibiofilm CDs based on recent development.

Mussel-inspired polymer with catechol and cationic Lys functionalities for dentin wet bonding.

Mussels can form tough and long-lasting adhesions to organic and inorganic surfaces in saline and impactive severe aquatic environments. Similar to mussel adhesion, dentin bonding occurs in a wet environment. However, unlike mussels, it is difficult to achieve long-lasting bonds with dentin. Moreover, water is considered a major hindrance in dentin bonding. Inspired by the synergistic effect of cationic lysine (Lys) and catechol on the elimination of the hydration layer during mussel adhesion, a catechol- and Lys-functionalized polymerizable polymer (catechol-Lys-methacrylate [CLM]) was synthesized to replicate the complex synergy between amino acids and catechol. The bond-promoting potential of 5 â€‹mg/mL CLM primer was confirmed using an in vitro wet dentin-bonding model, which was characterized by an improvement in bond strength and durability. CLM can adhere to wet demineralized dentin, with Lys acting as a molecular vanguard to expel water. Subsequently, a myriad of interfacial interactions can be obtained by introducing the catechol group into the interface. Additionally, tough and long-lasting adhesion, similar to that formed by mussels, can be achieved by grafting CLM onto type I collagen via covalent bonds, hydrogen bonds, Van der Waals interactions, and cation-π interactions, which can enhance the mechanical and chemical stability of collagen, increase the enzymatic resistance of collagen, and provide additional physical/chemical adhesion to dentin bonds. Catechol- and cationic Lys-functionalized polymers can improve the stability of the resin-dentin interface under wet conditions.

Cytocompatible Amphipathic Carbon Quantum Dots as Potent Membrane-Active Antibacterial Agents with Low Drug Resistance and Effective Inhibition of Biofilm Formation.

It is very challenging to design nanomaterials with both excellent antibacterial activity and cytocompatibility when facing bacterial infection. Here, inspired by antimicrobial peptides (AMPs), we fabricate carbon quantum dots (CQDs) derived from hydrophobic tryptophan and hydrophilic lysine or arginine (Lys/Trp-CQDs and Arg/Trp-CQDs), which possess amphipathic properties. These CQDs could effectively destroy bacterial membranes without developing resistance, inhibit biofilms formed by Staphylococcus aureus, and exhibit good in vitro biocompatibility. The antibacterial activities are caused by not only surface cationic structures and excess intracellular reactive oxygen species (ROS) generated by the CQDs but also the effects of the surface hydrophobic groups. These combined mechanisms of actions lead to bacterial membrane disruption, which raises the hope for combating bacterial infection without concern about drug resistance. What's more, the effect of amphiphilicity on balancing sterilization with biocompatibility expands the research ideas for developing available antibacterial nanomaterials.

Photothermal-enhanced antibacterial and antioxidant hydrogel dressings based on catechol-modified chitosan-derived carbonized polymer dots for effective treatment of wound infections.

Bacterial infection and excessive reactive oxygen species (ROS) remain challenging factors contributing to the delayed healing of chronic wounds. Although various antibacterial and antioxidant hydrogel dressings have been developed to accelerate wound healing, multifunctional hydrogels fabricated by rationally designing and introducing carbonized polymer dots (CPDs) have rarely been reported. Herein, inspired by the mussel biomimetic approach, we synthesized 3,4-dihydroxybenzaldehyde functionalized chitosan (DFC), and then the polymeric precursor was pyrolyzed into CPDs with abundant amino and catechol groups on the surface, which endowed it with a highly positively charged surface that could activate the photothermal effect under near-infrared (NIR) light irradiation. Finally, the nanocomposite hydrogel (PVA@CPDs) was simply constructed by directly mixing polyvinyl alcohol (PVA) with CPDs, utilizing the freeze-thaw cycle method to form a gel, in which, CPDs as a center of polyfunctional nanoparticles drove the formation of PVA microcrystalline crosslinking and endowed the PVA substrate with versatile functionalities. Remarkable and comprehensive improvements in the swelling behavior, mechanical properties and adhesive strength of the hydrogel could be conveniently achieved with the suitable loading of CPDs. The in vitro experiments demonstrated that the PVA@CPDs hydrogel presented broad-spectrum and rapid bactericidal activity, concurrently acting as an effective antioxidant being able to scavenge free radicals. In addition, no obvious cytotoxicity was observed for the multifunctional hydrogel after incubation with L02 cells. In vivo evaluation in an infected full-thickness skin wound model demonstrated that the PVA@CPDs hydrogel promoted wound closure without any side effects. As a consequence, the current work manifests a facile yet versatile strategy to develop effective and biocompatible multifunctional hydrogel dressings for bacteria-infected wound healing.

Acid-activated ROS generator with folic acid targeting for bacterial biofilm elimination.

Many medical and chemical applications require the precise supply of antimicrobial components in a controlled manner at the location of mature biofilm deposits. This work reports a facile strategy to fabricate nanoscale metal-organic frameworks (NMOFs) coencapsulating the antibacterial ligand (lysine carbon dots, Lys-CDs) and targeted drug (folic acid, FA) in one pot to improve antibiofilm efficiency against established biofilms. The resulting products are characterized by transmission electron microscopy, field-emission scanning electron microscopy, powder x-ray diffraction, and ultraviolet-visible spectroscopy. The results show that Lys-CDs could coordinate with Zn2+ and the adding of FA inhibits the coordination of Lys-CDs with central ions of Zn. The Lys-CDs and FA are successfully exposed with the NMOFs disintegrating in the acid environment of bacterial metabolites. We are surprised to find a sharp increase of reactive oxygen species (ROS) inside the bacterial cells by FA functionalizing NMOFs, which undoubtedly enhance the antibacterial and antibiofilm activity. The as-synthesized ZIF-8-based nanocomposites also show the peroxidase-like activity in an acid environment, and produce extremely active hydroxyl radicals resulting in the improved antibacterial and antibiofilm activity. The possible mechanisms of antibacterial activities indicate that the presence of FA is significant in the sense of targeting bacteria. This study shows a novel approach to construct acid stimulation supply system which may be helpful for the research of antibiofilms.

A facile injectable carbon dot/oxidative polysaccharide hydrogel with potent self-healing and high antibacterial activity.

Bacterial infection is one of the most formidable problems in wound healing, which inflicts severe pain on patients while causing wound ulceration. Here, we prepared an injectable self-healing carbon dot hydrogel with outstanding antibacterial activity only using ε-poly(L-lysine) carbon dot (PL-CD) and oxidized dextran (ODA). The particle size of PL-CD prepared by pyrolysis of poly-l-lysine was about 3 nm. Moreover, PL-CD with abundant -NH2 on its surface could not only act as nodes to connect ODA through Schiff base to construct PL-CD@ODA hydrogel network, but also offer excellent antibacterial properties. As the contacting and releasing antibacterial action of the PL-CD@ODA hydrogel, nearly 100 % of the 107 CFU/mL of S. aureus was killed after 10 min of contacting. In addition, PL-CD@ODA hydrogel showed flexible injectability and extremely strong self-healing properties after being severely damaged. When 1000 % shear stress applied to the hydrogel, complete healing could be achieved within a few seconds.