Few studies aiming to develop a glue with an underwater reusable adhesive property have been reported because combining the two properties of reusable adhesion and underwater adhesion into a single glue formulation is a challenging issue. Herein, preparation of a simple mixture of poly(vinyl alcohol) (PVA) and a well-known phenolic compound, namely, tannic acid (TA), results in an underwater glue exhibiting reusable adhesion. We named the adhesive VATA (PVA + TA). Using VATA, two stainless steel objects (0.77 kg each) are able to be instantly attached. In addition to the high adhesive strength, surface-applied VATA in water retains its adhesive capability even after 24 h. In contrast, cyanoacrylate applied under the same water condition rapidly loses its adhesive power. Another advantage is that VATA's adhesion is reusable. Bonded objects can be forcibly detached, and then the detached ones can be reattached by the residual VATA. VATA maintains nearly 100% of its initial adhesive force, even after 10 repetitions of attach−detach cycles. VATA bonds various materials ranging from metals and polymers to ceramics. Particularly, we first attempt to test the toxicity of the underwater adhesives using an invertebrate nematode, Caenorhabditis elegans and gold fish (vertebrate) due to potential release to the environment.

Mussel-inspired adhesive coatings on biomedical devices have attracted significant interest due to their unique properties such as substrate independency and high efficiency. The key molecules for mussel-inspired adhesive coatings are catechol and amine groups. Along with the understanding of catechol chemistry, chitosan-catechol has also been developed as a representative mussel-inpired adhesive polymer that contains catechol and amine groups for adhesiveness. Herein, we demonstrated the direct writability of chitosan-catechol as a bioink for 3D printing, one of the additive techniques. The use of chitosan-catechol bioink results in the formation of 3D constructs in normal culture media via rapid complexation of this bioink with serum proteins; in addition, the metal/catechol combination containing tiny amounts of vanadyl ions, in which the ratio of metal to catechol is 0.0005, dramatically enhances the mechanical strength and printability of the cell-encapsulated inks, showing a cell viability of approximately 90%. These findings for mussel-inspired bioinks will be a promising way to design a biocompatible 3D bioink cross-linked without any external stimuli.

Catechol-containing hydrogels have been exploited in biomedical fields due to their adhesive and cohesive properties, hemostatic abilities, and biocompatibility. Catechol moieties can be oxidized to o-catecholquinone, a chemically active intermediate, in the presence of oxygen to act as an electrophile to form catechol-catechol or catechol-amine/thiol adducts. To date, catechol cross-linking chemistry to fabricate hydrogels has been mostly performed at room temperature. Herein, we report large increases in catechol crosslinking reaction kinetics by the freeze−thawing process. The formation of ice crystals during freezing steps spatially condenses catechol-containing polymers into nearly frozen (yet unfrozen) regions, resulting in decreases in the polymeric chain distances. This environment allows great increases in catechol cross-linking kinetics, a phenomenon that can also occur during thawing steps. The increased cross-linking rate and spatial condensation in the cryogels provide unique wall and pore structures, which result in elastic, spongelike hydrogels. The moduli of the cryogels prepared by glycol-chitosan-catechol (g-chitosan-c) were improved by 3−6-fold compared to room temperature-cured conventional hydrogels, and the degree of improvement increased depending on the freezing time and the number of freeze−thawing cycles. Unlike typical cell encapsulations before cross-linking, which have often been a source of cytotoxicity, the macroporosity of cryogels allows nontoxic cell seeding with ease. This research offers a new way to utilize catechol cross-linking chemistry by freeze−thawing processes to simultaneously regulate mechanical strength and porous structures in catechol-containing hydrogels.

Infectious bacteria evolve fast into resistance to conventional antimicrobial agents, whereas treatments for drug resistance bacteria progress more slowly. Here, we report a universally applicable photoactivated antimicrobial modality through light-responsive carbon dot-embedding soft hyaluronic acid hydrogel (CDgel). Because of the innate nature of the infectious bacteria that produce hyaluronidase, applied hyaluronic acid-based CDgel breaks down via bacteria and releases carbon dots (CDs) into the infectious sites. The released CDs possess photodynamic capabilities under light irradiation, inducing 1O2 generation and growth inhibition of the infectious bacteria, S. aureus and E. coli (∼99% and ∼97%, respectively), in vitro. In particular, these photodynamic effects of CDs from CDgel have been shown to accelerate the healing of infected wounds in vivo, showing a higher wound regeneration rate as compared to that of untreated wounds. Our work demonstrates that the biocompatible and shape-controllable CDgel possesses therapeutic potential as a treatment modality for the light-driven control of drug-resistant bacterial infections.

Liquid–liquid phase separation in an aqueous polymer solution is a unique physicochemical phenomenon, and the material present in the dense bottom layer is called a coacervate. A partial degree of water exclusion during coacervate formation often results in adhesive properties. The high viscosity makes coacervates incompatible with electrospinning processes. Coacervates can be electrospinnable only when the viscosity level of coacervates is adjusted. Electrospinning of coacervates results in a liquid-to-solid phase transition, addressing a long-term stability issue of coacervates. The preserved electrospun membranes can always be reconverted to a coacervate state by dissolution. Herein, we fabricate a spinnable coacervate solution using cosolvents. For neutral, hydrogen bond-dominated coacervates, such as those composed of poly­(vinyl alcohol) (PVA) and phenolic tannic acid (TA), the use of a polar cosolvent system such as methanol–water results in an electrospinnable coacervate solution. The spun PVA–TA porous mats are a physicochemically stable solid, and the materials are converted back to an adhesive state upon wetting with body fluid. Considering the emerging studies related to coacervate adhesives, this study suggests that electrospinning a coacervate solution can be a strategy to dramatically increase the material stability and functionality.

We introduce a nature-inspired coating for SEM imaging of hydrated soft biomaterials by aerobic oxidation of polyphenols.

Silicosis is an irreversible and progressive fibrotic lung disease caused by massive inhalation of crystalline silica dust at workplaces, affecting millions of industrial workers worldwide. A tyrosine kinase inhibitor, nintedanib (NTB), has emerged as a potential silicosis treatment due to its inhibitory effects on key signaling pathways that promote silica‐induced pulmonary fibrosis. However, chronic and frequent use of the oral NTB formulation clinically approved for treating other fibrotic lung diseases often results in significant side effects. To this end, we engineered a nanocrystal‐based suspension formulation of NTB (NTB‐NS) possessing specific physicochemical properties to enhance drug retention in the lung for localized treatment of silicosis via inhalation. Our NTB‐NS formulation was prepared using a wet‐milling procedure in presence of Pluronic F127 to endow the formulation with nonadhesive surface coatings to minimize interactions with therapy‐inactivating delivery barriers in the lung. We found that NTB‐NS, following intratracheal administration, provided robust anti‐fibrotic effects and mechanical lung function recovery in a mouse model of silicosis, whereas a 100‐fold greater oral NTB dose given with a triple dosing frequency failed to do so. Importantly, several key pathological phenotypes were fully normalized by NTB‐NS without displaying notable local or systemic adverse effects. Overall, NTB‐NS may open a new avenue for localized treatment of silicosis and potentially other fibrotic lung diseases.

Recently, miraculous therapy approaches involving adeno-associated virus (AAV) for incurable diseases such as spinal muscular atrophy and inherited retinal dysfunction have been introduced. Nonreplicative, nonpathogenic, low rates of chromosome insertional properties and the existence of neutralizing antibodies are main safety reasons why the FDA approved its use in gene delivery. To date, AAV production always results in a mixture of nontherapeutic (empty) and therapeutic (DNA-loaded) full capsids (10–98%). Such existence of empty viral particles inevitably increases viral doses to human. Thus, the rapid monitoring of empty capsids and reducing the empty-to-full ratio are critical in AAV science. However, transmission electron microscopy (TEM) is the primary tool for distinguishing between empty and full capsids, which creates a research bottleneck because of instrument accessibility and technical difficulty. Herein, we demonstrate that atomic force microscopy (AFM) can be an alternative tool to TEM. The simple, noncontact-mode imaging of AAV particles allows the distinct height difference between full capsids (∼22 nm) and empty capsids (∼16 nm). The sphere-to-ellipsoidal morphological distortion observed for empty AAV particles clearly distinguishes them from full AAV particles. Our study indicates that AFM imaging can be an extremely useful, quality-control tool in AAV particle monitoring, which is beneficial for the future development of AAV-based gene therapy.