Insect cuticle-inspired design of sustainably sourced composite bioplastics with enhanced strength, toughness and stretch-strengthening behavior.

Insect cuticles that are mainly made of chitin, chitosan and proteins provide insects with rigid, stretchable and robust skins to defend harsh external environment. The insect cuticle therefore provides inspiration for engineering biomaterials with outstanding mechanical properties but also sustainability and biocompatibility. We herein propose a design of high-performance and sustainable bioplastics via introducing CPAP3-A1, a major structural protein in insect cuticles, to specifically bind to chitosan. Simply mixing 10w/w% bioengineered CPAP3-A1 protein with chitosan enables the formation of plastics-like, sustainably sourced chitosan/CPAP3-A1 composites with significantly enhanced strength (∼90 MPa) and toughness (∼20 MJ m -3), outperforming previous chitosan-based composites and most synthetic petroleum-based plastics. Remarkably, these bioplastics exhibit a stretch-strengthening behavior similar to the training living muscles. Mechanistic investigation reveals that the introduction of CPAP3-A1 induce chitosan chains to assemble into a more coarsened fibrous network with increased crystallinity and reinforcement effect, but also enable energy dissipation via reversible chitosan-protein interactions. Further uniaxial stretch facilitates network re-orientation and increases chitosan crystallinity and mechanical anisotropy, thereby resulting in stretch-strengthening behavior. In general, this study provides an insect-cuticle inspired design of high-performance bioplastics that may serve as sustainable and bio-friendly materials for a wide range of engineering and biomedical application potentials.

An All-in-One Tannic Acid-Containing Hydrogel Adhesive with High Toughness, Notch Insensitivity, Self-Healability, Tailorable Topography, and Strong, Instant, and On-Demand Underwater Adhesion.

Hydrogels that are mechanically tough and capable of strong underwater adhesion can lead to a paradigm shift in the design of adhesives for a variety of biomedical applications. We hereby innovatively develop a facile but efficient strategy to prepare hydrogel adhesives with strong and instant underwater adhesion, on-demand detachment, high toughness, notch-insensitivity, self-healability, low swelling index, and tailorable surface topography. Specifically, a polymerization lyophilization conjugation fabrication method was proposed to introduce tannic acid (TA) into the covalent network consisting of polyethylene glycol diacrylate (PEGDA) of substantially high molecular weight. The presence of TA facilitated wet adhesion to various substrates by forming collectively strong noncovalent bonds and offering hydrophobicity to allow water repellence and also provided a reversible cross-link within the binary network to improve the mechanical performance of the gels. The long-chain PEGDA enhanced the efficacy and stability of TA conjugation and contributed to gel mechanics and adhesion by allowing chain diffusion and entanglement formation. Moreover, PEGDA/TA hydrogels were demonstrated to be biocompatible and capable of accelerating wound healing in a skin wound animal model as compared to commercial tissue adhesives and can be applied for the treatment of both epidermal and intracorporeal wounds. Our study provides new, critical insight into the design principle of all-in-one hydrogels with outstanding mechanical and adhesive properties and can potentially enhance the efficacy of hydrogel adhesives for wound healing.

Ag nanoparticles decorated electrospinning carbon nanotubes/polyamide nanofibers.

Antibacterial composite nanofibers have recently been widely applied in biomedical fields. The purpose of this study is to combine Polyamide66 (PA) with carbon nanotubes (CNTs) and Ag nanoparticles through electrospinning and the aqueous reduction method to synthesis Ag@CNT/PA composite nanofibers with excellent conductivity, antibacterial property and cytocompatibility. The morphology and structure of Ag@CNT/PA composite nanofibers were analyzed by a series of characterizations. Conductivity of Ag@CNT/PA composite nanofibers in wet state was measured using a four-probe resistance tester. The antibacterial activity of Ag@CNT/PA composite nanofibers was tested by inhibition zone method, and the MG-63 cells were used to detect the cytotoxicological effects of the composite nanofibers. The results show that the Ag nanoparticles (50-100 nm) are distributed uniformly on the surface of nanofibers. Conductivity of Ag@CNT/PA composite nanofibers reaches (9.918 ± 0.043) × 10-4 S mm-1, significantly higher than that of PA nanofibers ((1.486 ± 0.017) × 10-4 S mm-1). The Ag@CNT/PA composite fibers present good antibacterial activity against Escherichia coli and Staphylococcus aureus. Cell culture results show that the cell proliferation of Ag@CNT/PA composite nanofiber group seems no significant difference with PA nanofiber group (p > 0.05) at day 7. The Ag@CNT/PA composite nanofibers have no significant negative effects on MG-63 cells.

Preparation and characterization of porous hydroxyapatite/ß-cyclodextrin-based polyurethane composite scaffolds for bone tissue engineering.

In this study, novel porous scaffolds containing hydroxyapatite and ß-cyclodextrin-based polyurethane were first successfully fabricated by polymerizing ß-cyclodextrin with hexamethylene diisocyanate and hydroxyapatite in situ for bone tissue engineering. The physicochemical and mechanical properties as well as cytocompatibility of porous scaffolds were investigated. The results showed that polyurethane reinforced with hydroxyapatite composites had cancellous bone-like porous structure. The mechanical strength of the scaffolds increased with increasing the hydroxyapatite content in scaffolds. Synthesized scaffolds (PU1, PUHA1, PU2, and PUHA2) presented compressive strength values of 0.87 ± 0.24 MPa, 1.81 ± 0.10 MPa, 6.16 ± 0.89 MPa, and 12.95 ± 2.05 MPa, respectively. The pore size and porosity of these scaffolds were suitable for bone regeneration. Cytocompatibility of composite scaffolds was proven via favorable interactions with MC3T3-E1 cells. The addition of hydroxyapatite into CD-based polyurethane scaffolds improved cell attachment, well-spread morphology, and higher proliferation. The hydroxyapatite-polyurethane scaffolds have the potential to be applied in bone repair and regeneration.

Effect of hydroxyapatite fillers on the mechanical properties and osteogenesis capacity of bio-based polyurethane composite scaffolds.

A newly designed hydroxyapatite-polyurethane (HA-PU) composite scaffold was prepared by polymerizing glyceride of castor oil (GCO) with isophorone diisocyanate (IPDI) and HA as fillers. The aim of this study was to determine the effect of HA fillers on the mechanical properties and osteogenesis capacity of the composite scaffolds. The physical and biological properties of the scaffold were evaluated by SEM observation, mechanical testing, cell culture and animal experiments. The results showed that HA fillers enhanced the mechanical properties of PU composite scaffolds such as compressive strength and elastic modulus. The mechanical properties of the scaffolds were seen to increase with increase in HA loading. The compressive strength of composite scaffold with 0 wt%, 20 wt%, 40 wt% of HA was 0.6 ±â€¯0.1 MPa, 2.1 ±â€¯0.1 MPa, and 4.6 ±â€¯0.3 MPa, respectively. In vitro biodegradation studies of scaffolds were carried out. The results showed that all of the scaffolds were susceptible to cholesterol esterase (CE) -catalyzed degradation. HA-PU composite scaffolds exhibited a high affinity to osteoblastic cells and were good template for cell growth and proliferation. When implanted in bone defects of rats, PU scaffolds incorporated HA were biocompatible with the tissue host and had no immune rejection. Moreover, the higher the loading of HA in the composite scaffold, the better chances of osteogenesis. It confirmed that the prepared HA-PU composite scaffolds can be promising candidate for bone repair and bone tissue engineering.