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Next-generation structural materials are expected to be lightweight, high-strength and tough composites with embedded functionalities to sense, adapt, self-repair, morph and restore. This Review highlights recent developments and concepts in bioinspired nanocomposites, emphasizing tailoring of the architecture, interphases and confinement to achieve dynamic and synergetic responses. We highlight cornerstone examples from natural materials with unique mechanical property combinations based on relatively simple building blocks produced in aqueous environments under ambient conditions. A particular focus is on structural hierarchies across multiple length scales to achieve multifunctionality and robustness. We further discuss recent advances, trends and emerging opportunities for combining biological and synthetic components, state-of-the-art characterization and modelling approaches to assess the physical principles underlying nature-inspired design and mechanical responses at multiple length scales. These multidisciplinary approaches promote the synergetic enhancement of individual materials properties and an improved predictive and prescriptive design of the next era of structural materials at multilength scales for a wide range of applications.This Review discusses recent progress in bioinspired nanocomposite design, emphasizing the role of hierarchical structuring at distinct length scales to create multifunctional, lightweight and robust structural materials for diverse technological applications.

Inverse vulcanization of waste or renewable dienes has generated materials with phenomenal properties across a spectrum of applications. Nevertheless, the use of these materials for structural applications remains a challenge. Here, the use of an inverse vulcanized cyclopentadiene polymer as a resin for carbon fiber reinforced composites is explored. The dynamic S─S bonds in the polymer matrix are used to repair composite specimens over 5 generations by heating the material to 140 °C. A range of composites are manufactured and evaluated for their flexural properties, using a range of fiber orientations. Finally, this polymer is used to reinforce a carbon fiber fabric composed entirely of reclaimed materials, constituting a composite entirely composed of waste materials and second life carbon fibers. With the ability to synthesis shelf stable, rehealable sulfur‐based copolymers in hand, this paper aims to highlight a means to improve their structural integrity using carbon fiber reinforcements in hopes to further widen the scope of applications these polymers can have. Furthermore, the repair capabilities of these composites over 5 consecutive generations are assessed and reported.

Nature has evolved to create materials of unmatched performance governed by the interfacial interactions between hard and soft surfaces. Typically, in a carbon fibre composite, one polymer and one type of carbon fibre is used throughout a laminate. In this work, we use a carbon fibre surface modification approach to vary the fibre–matrix interface throughout the laminate to tailor the soft–hard interfaces. We demonstrate this effect using reclaimed carbon fibre materials in a thermoset polymer, then extend this concept to a thermoplastic polymer matrix–polypropylene. The thermoset specimens examined in this work consist of 5 carbon fibre plies, featuring 0, 1, 3 or 5 surface-modified layers located at the centre of the composite. The largest improvements in physical properties for these composites (yield strength, ultimate flexural strength, and tensile modulus) were found when only 1 modified layer of carbon fibre was placed directly within the centre of the composite. Subsequent investigations revealed that for a polypropylene matrix, where the surface chemistry is tailored specifically for polypropylene, improvements are also observed when mixed surface chemistries are used. This work shows that surface modification of reclaimed carbon fibres as non-woven mats can provide significant improvements in mechanical properties performance for structural composites when used in strategically advantageous locations throughout the composite.

Conductive fibers are needed for the development of flexible electronic and biomedical devices. MXene fibers show great promise for use in such applications because of their high conductivity. Current literature on MXene fiber development highlights the need for improving their mechanical properties and investigation of biocompatibility. Here the use of silk fibroin biopolymer as a MXene formulation additive for the production of MXene fibers is studied. It is found that the favorable silk fibroin–MXene interactions resulted in improved durability, withstanding up to 1 h of high frequency sonication in buffered solutions. Furthermore, fibers with ≈5 wt% silk fibroin displays interesting properties including high conductivity (≈3700 S cm−1), high volumetric capacitance (≈910 F cm−3), and non‐cytotoxicity toward THP‐1 monocytic cells. The results presented here provide an important insight into potential use of MXene fibers in flexible electronics and biomedical applications. A new investigation of MXene–silk fibroin composite fibers is presented. The favorable interfacial interactions between silk and MXene resulted in outstanding mechanical and electrical properties. Their biocompatibility provides an important insight into their potential use in flexible electronics and biomedical applications.

Bonding dissimilar materials has been a persistent challenge for decades. This paper presents a method to modify a stainless steel surface (316 L), routinely used in medical applications to enable the significant adhesion of a biopolymer (silk fibroin). The metallic surface was first covalently grafting with polyacrylamide, to enable a hydrogen bonding compatible surface. The polymerisation was initiated via the irreversible electrochemical reduction of a 4‐nitrobenzene diazonium salt (20 mM), in the presence of an acrylamide monomer (1 M) at progressively faster scan rates (0.01 V/s to 1 V/s). Examination of the modified samples by FT‐IR was consistent with successful surface modification, via observations of the acrylamide carbonyl (1600–1650 cm−1) was observed, with more intense peaks correlating to slower scan rates. Similar observations were made with respect to increasing surface polarity, assessed by water contact angle. Reductions of >60° were observed for the grafted surfaces, relative to the unmodified control materials, indicating a surface able to undergo significant hydrogen bonding. The adhesion of silk to the metallic surface was quantified using a lap shear test, effectively using silk fibroin as an adhesive. Adhesion improvements of 5–7‐fold, from 4.1 MPa to 29.3 MPa per gram of silk fibroin, were observed for the treated samples, highlighting the beneficial effect of this surface treatment. The methods developed in this work can be transferred to any metallic (or conductive) surface and can be tailored to complement any desired interface. The adhesion of silk fibroin to stainless steel was enhanced by electrografting polyacrylamide polymer on to the metallic surface. Adhesion of the silk fibroin to the stainless steel was evaluated using lap‐shear testing, with up to 7x improvement in ahdesion observed.

Background Solvate ionic liquids (SILs) are a new class of ionic liquids that are equimolar solutions of lithium bistrifluoromethanesulfonimide in either triglyme or tetraglyme, referred to as G3LiTFSA and G4LiTFSA, respectively. SILs play a role in energy storage lithium batteries, and have been proposed as potential alternatives to traditional organic solvents such as DMSO. G3TFSA and G4TFSA have been shown to exhibit no toxicity in vivo up to 0.5% (v/v), and solubilize small compounds (N,N-diethylaminobenzaldehyde) with full penetrance, similar to DMSO delivered DEAB. Herein, we compare the effects of storage (either at room temperature or − 20 °C) on DEAB solubilized in either DMSO, G3TFSA or G4TFSA to investigate compound degradation and efficacy. Results The findings show that DEAB stored at room temperature (RT) for 4 months solubilized in either G3TFSA, G4TFSA or DMSO displayed no loss of penetrance. The same was observed with stock solutions stored at − 20 °C for 4 months; however G4TFSA remained in a liquid state compared to both G3TFSA and DMSO. Moreover, we examined the ability of G3TFSA and G4TFSA to solubilize another small molecular therapeutic, the FGFR antagonist SU5402. G4TFSA, unlike G3TFSA solubilized SU5402 and displayed similar phenotypic characteristics and reduced dlx2a expression as reported and shown with SU5402 in DMSO; albeit more penetrative. Conclusion This study validates the use of these ionic liquids as a potential replacement for DMSO in vivo as organic solubilizing agents.

Thermally conductive polyvinylidene fluoride (PVDF) composites were prepared by incorporating carbon fibers (CFs) with different lengths (286.6 ± 7.1 and 150.0 ± 2.3 µm) via cold pressing, followed by sintering. The length effects of the CF on the thermal conductivity, polymer crystallization behaviors, and mechanical properties of the PVDF composites were studied. The through-plane thermal conductivity of the PVDF composites increased significantly with the rise in CF loadings. The highest thermal conductivity of 2.89 W/(m∙K) was achieved for the PVDF composites containing 40 wt.% shorter CFs, ~17 times higher than that of the pure PVDF (~0.17 W/(m∙K)). The shorter CFs had more pronounced thermal conductive enhancement effects than the original longer CFs at higher filler loadings. CFs increased the storage modulus and the glass transition temperature of the PVDF. This work provides a new way to develop thermally conductive, mechanically, and chemically stable polymer composites by introducing CFs with different lengths.

Here we report on how residence time influences the evolution of the structure and properties through each stage of the carbon fibre manufacturing process. The chemical structural transformations and density variations in stabilized fibres were monitored by Fourier Transform Infrared Spectroscopy and density column studies. The microstructural evolution and property variation in subsequent carbon fibres were studied by X-ray diffraction and monofilament tensile testing methods, which indicated that the fibres thermally stabilized at longer residence times showed higher degrees of structural conversion and attained higher densities. Overall, the density of stabilized fibres was maintained in the optimal range of 1.33 to 1.37 g/cm3. Interestingly, carbon fibres manufactured from higher density stabilized fibres possessed lower apparent crystallite size (1.599 nm). Moreover, the tensile strength of carbon fibres obtained from stabilized fibres at the high end of the observed range (density: 1.37 g/cm3) was at least 20% higher than the carbon fibres manufactured from low density (1.33 g/cm3) stabilized fibres. Conversely, the tensile modulus of carbon fibres produced from low density stabilized fibres was at least 17 GPa higher than those from high density stabilized fibres. Finally, it was shown that there is potential to customize the required properties of resultant carbon fibres suiting specific applications via careful control of residence time during the stabilization stage.

This work demonstrates the introduction of various α-aminophosphonate compounds to an epoxy resin system, thereby improving flame retardance properties. The α-aminophosphonate scaffold allows for covalent incorporation (via the secondary amine) of the compounds into the polymer network. This work explores the synergistic effect of phosphorus and halogens (such as fluorine) to improve flame retardancy. The compounds were all prepared and isolated in analytical purity and in good yield (95%). Epoxy samples were prepared, individually incorporating each compound. Thermogravimetric analysis showed an increased char yield, indicating an improved thermal resistance (with respect to the control sample). Limiting oxygen index for the control polymer was 28.0% ± 0.31% and it increased to 34.6% ± 0.33% for the fluorinated derivative.

Silk fibroin interactions with metallic surfaces can provide utility for medical materials and devices. Toward this goal, titanium alloy (Ti6Al4 V) was covalently grafted with polyacrylamide via electrochemically reducing 4‐nitrobenzene diazonium salt in the presence of acrylamide. Analysis of the modified surfaces with FT‐IR spectra, SEM and AFM were consistent with surface grafting. Functionalised titanium samples with a silk fibroin membrane, with and without impregnated therapeutics, were used to assess cytocompatibility and drug delivery. Initial cytocompatibility experiments using fibroblasts showed that the functionalised samples, both with and without silk fibroin coatings, supported significant increases between 72–136 % in cell metabolism, compared to the controls after 7 days. A 7‐days release profiling showed consistent bacterial inhibition through gentamicin release with average inhibition zones of 239 mm2. Over a 5‐week period, silk fibroin coated samples, both with and without growth factors, supported better human mesenchymal stem cell metabolism with increases reaching 1031 % and 388 %, respectively, compared to samples without the silk fibroin coating with. A titanium alloy (Ti6Al4 V) was covalently grafted with polyacrylamide in preparation for its modification with a silk fibroin membrane. The functionalised samples with and without impregnated therapeutics were used to assess cytocompatibility and drug delivery. Over a 5‐week period, silk fibroin‐coated samples, both with and without loaded growth factors, supported better human mesenchymal stem cell metabolism compared to samples without the silk fibroin coating.