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The occurrence of osteoarthritis (OA) is highly associated with the reduced lubrication property of the joint, where a progressive and irreversible damage of the articular cartilage and consecutive inflammatory response dominate the mechanism. In this study, bioinspired by the super-lubrication property of cartilage and catecholamine chemistry of mussel, we successfully developed injectable hydrogel microspheres with enhanced lubrication and controllable drug release for OA treatment. Particularly, the lubricating microspheres (GelMA@DMA-MPC) were fabricated by dip coating a self-adhesive polymer (DMA-MPC, synthesized by free radical copolymerization) on superficial surface of photo-crosslinked methacrylate gelatin hydrogel microspheres (GelMA, prepared via microfluidic technology), and encapsulated with an anti-inflammatory drug of diclofenac sodium (DS) to achieve the dual-functional performance. The tribological test and drug release test showed the enhanced lubrication and sustained drug release of the GelMA@DMA-MPC microspheres. In addition, the functionalized microspheres were intra-articularly injected into the rat knee joint with an OA model, and the biological tests including qRT-PCR, immunofluorescence staining assay, X-ray radiography and histological staining assay all revealed that the biocompatible microspheres provided significant therapeutic effect against the development of OA. In summary, the injectable hydrogel microspheres developed herein greatly improved lubrication and achieved sustained local drug release, therefore representing a facile and promising technique for the treatment of OA.

Research into toughening an epoxy resin using biobased modifiers without trade-offs in its modulus, mechanical strength, and other properties still remains a challenge. In this article, an approach to toughen epoxy resin with tannic acid, a common polyphenolic compound extracted from plants and microorganisms, is presented. First, dodecane functionalized tannic acid (TA-DD) is prepared and subsequently incorporated into epoxy/anhydride curing system. Owing to the modification of long aliphatic chain, TA-DD can induce epoxy matrix yielding phase separation, forming microscaled separated phases. In the meantime, the terminal hydroxyl groups of TA-DD can participate in the curing process, which offers a good interfacial interaction between TA-DD and epoxy matrix. With such a mechanism, the results show that TA-DD can significantly toughen the epoxy resin without trade-offs in its strength, modulus, and T g . The thermoset with only 0.5 wt % TA-DD reaches highest impact strength, which is 196% increase of that of neat epoxy. This article opens up the possibility of utilizing the renewable tannic acid as an effective modifier for epoxy resin with good mechanical and thermal properties.

Specific recognition and separation of glycoproteins from complex biological solutions is very important in clinical diagnostics considering the close relationship between glycoproteins with the occurrence of diverse diseases, but the lack of materials with high selectivity and superior capture capacity still makes it a challenge. In this work, graphene oxide (GO) based molecularly imprinted polymers (MIPs) possessing double recognition abilities have been synthesized and applied as highly efficient adsorbents for glycoprotein recognition and separation. Boronic acid functionalized graphene oxide (GO-APBA) was first prepared and a template glycoprotein (ovalbumin, OVA) was then immobilized onto the surface of GO-APBA through boronate affinity. An imprinting layer was subsequently deposited onto GO-APBA surface by a sol-gel polymerization of organic silanes in aqueous solution. After the removal of the template glycoprotein, 3D cavities with double recognition abilities toward OVA were obtained in the as-prepared imprinted materials (GO-APBA/MIPs) because of the combination of boronate affinity and molecularly imprinted spatial matched cavities. The obtained GO-APBA/MIPs exhibited superior specific recognition toward OVA with imprinted factor (α) as high as 9.5, significantly higher than the corresponding value (4.0) of GO/MIPs without the introduction of boronic acid groups. Meanwhile, because of the synergetic effect of large surface area of graphene and surface imprinting, high binding capacity and fast adsorption/elution rate of GO-APBA/MIPs toward OVA were demonstrated and the saturation binding capacity of GO-APBA/MIPs could reach 278 mg/g within 40 min. The outstanding recognizing behavior (high adsorption capacity, highly specific recognition, and rapid binding rate) coupled to the facile and environmentally friendly preparation procedure makes GO-APBA/MIPs promising in the recognition, separation, and analysis of glycoproteins in clinics in the future.

A simple and green route was demonstrated to prepare graphene/Au NPs nanocomposite using polydopamine as surface modifier, reducing agent and stabilizer simultaneously, which exhibits remarkable catalytic activity for the reduction of 4-nitrophenol.

A series of biobased UV-curable antibacterial resins were synthesized through modifying tannic acid (TA) with varied amount of glycidyl methacrylate (GMA). The obtained TA-based methacrylates exhibited good film-forming property and can be cross-linked under UV irradiation. Thus, antibacterial functionalities can be tethered in the coating matrix, eliminating the loss of antibacterial ingredients. The antibacterial properties of resins and corresponding coatings against Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli were tested. The resins with high content of phenolic hydroxyl groups retained strong antibacterial ability while the ones with a relatively low content of phenolic hydroxyl groups did not, which indicated that the antimicrobial effects of TA greatly depended on the content of phenolic hydroxyl groups. The applications of UV-curable antibacterial resins in coatings were also studied. The cured coatings of TA-G5 resins with the highest content of phenolic hydroxyl groups exhibited the highest antibacterial activity with 5 log reduction. The basic properties of UV-cured coatings were also fully characterized, and the results demonstrated that the novel UV-curable resins had potential applications in UV-curable antibacterial coatings.

Stimuli-responsive microcapsules, which can release the encapsulated payload under various environmental stimuli, have attracted great interests of the food, pharmaceutical, cosmetics, and agricultural fields in recent years. However, most reported responsive microcapsules normally have a single storage area and thus load/release only one type of payload under one stimulus. In this work, we fabricated a novel kind of multicompartmental intelligent microcapsule with two storage areas and independently controlled (preprogrammable) releasing behavior under different stimuli via rapid photopolymerization of Pickering emulsions. In our strategy, a temperature-sensitive polymeric (Nisopropyl acrylamide, pNIPAM) particle was prepared and loaded with Nile Red (NR), which was then employed as a Pickering emulsifier to stabilize oil-in-water droplets. The oil was composed of pH-responsive monomers and oil-soluble fluorescent green (OG). Upon exposure to photoirradiation, pH-responsive monomers were polymerized along the interior of the droplets and converted into microcapsules. With NR in the temperature-sensitive pNIPAM@NR particles and OG in the interior of the microcapsules, the as-prepared microcapsules possess dual-carrier capability with two payloads encapsulated dependently in two different compartments. In addition, the microcapsules could respond to two different external stimuli (temperature and pH) and realize the selective and independent release of encapsulated molecules (NR and OG) from the shell and core without any mutual interference. More importantly, the release of NR and OG can be programmed by preprogramming the order of the stimulus responses, which can be altered. Our work develops a simple and effective strategy to fabricate responsive multicompartment microcapsules with preprogrammable release of different molecules.

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