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Self-assembling natural drug hydrogels formed without structural modification and able to act as carriers are of interest for biomedical applications. A lack of knowledge about natural drug gels limits there current application. Here, we report on rhein, a herbal natural product, which is directly self-assembled into hydrogels through noncovalent interactions. This hydrogel shows excellent stability, sustained release and reversible stimuli-responses. The hydrogel consists of a three-dimensional nanofiber network that prevents premature degradation. Moreover, it easily enters cells and binds to toll-like receptor 4. This enables rhein hydrogels to significantly dephosphorylate IκBα, inhibiting the nuclear translocation of p65 at the NFκB signalling pathway in lipopolysaccharide-induced BV2 microglia. Subsequently, rhein hydrogels alleviate neuroinflammation with a long-lasting effect and little cytotoxicity compared to the equivalent free-drug in vitro. This study highlights a direct self-assembly hydrogel from natural small molecule as a promising neuroinflammatory therapy. There is interest in the development of drug-based hydrogels for responsive sustained drug release. Here, the authors report on the self-assembly of natural small molecule, rhein, into hydrogels and the application of the hydrogels as stable controlled release agents for neuro-inflammatory therapy

Mechanical responsiveness in many plants is produced by helical organizations of cellulose microfibrils. However, simple mimicry of these naturally occurring helical structures does not produce artificial materials with the desired tunable actuations. Here, we show that actuating fibres that respond to solvent and vapour stimuli can be created through the hierarchical and helical assembly of aligned carbon nanotubes. Primary fibres consisting of helical assemblies of multiwalled carbon nanotubes are twisted together to form the helical actuating fibres. The nanoscale gaps between the nanotubes and micrometre-scale gaps among the primary fibres contribute to the rapid response and large actuation stroke of the actuating fibres. The compact coils allow the actuating fibre to rotate reversibly. We show that these fibres, which are lightweight, flexible and strong, are suitable for a variety of applications such as energy-harvesting generators, deformable sensing springs and smart textiles. Lightweight, flexible and strong fibre actuators that respond to solvents and vapours are made by twisting together several well-aligned helical fibres of multiwalled carbon nanotubes.

Novel 2D Ti3C2Tx (MXene)-reinforced polyvinyl alcohol (PVA) nanofibers have been successfully fabricated by an electrospinning technique. The high aspect ratio, hydrophilic surfaces, and metallic conductivity of delaminated MXene nanosheet render it promising nanofiller for high performance nanocomposites. Cellulose nanocrystals (CNC) were used to improve the mechanical properties of the nanofibers. The obtained electrospun nanofibers had diameter from 174 to 194 nm depending on ratio between PVA, CNC and MXene. Dynamic mechanical analysis demonstrated an increase in the elastic modulus from 392 MPa for neat PVA fibers to 855 MPa for fibers containing CNC and MXene at 25°C. Moreover, PVA nanofibers containing 0.14 wt. % Ti3C2Tx exhibited dc conductivity of 0.8 mS/cm conductivity which is superior compared to similar composites prepared using methods other than electrospinning. Improved mechanical and electrical characteristics of the Ti3C2Tx /CNC/PVA composites make them viable materials for high performance energy applications.

How spiders' silk collects water The glistening of spiders' webs on a misty morning shows that they can gather water droplets from humid air with impressive efficiency. A study of the capture silk of the spider Uloborus walckenaerius reveals that this capability depends on a structural change that occurs on wetting. 'Wet-rebuilt' fibres are characterized by periodic spindle-knots made of random nanofibrils separated by joints made of aligned nanofibrils. This structure produces a surface energy gradient between the spindle-knots and the joints, and a difference in the pressure acting on drops in contact with either the spindle-knots or the joints. This ensures that water can continuously condense around the joints and is then transported to the spindle-knots, where it can accumulate in large hanging drops. An artificial silk mimicking the structure of wetted spider silk can also gather water drops from thin mist. This work could inform the design of functional surfaces that can collect fresh water from fog, or filter liquid aerosols in industrial processes. Many plants and animals make use of biological surfaces with structural features at the micro- and nanometre-scale that control the interaction with water. The appearance of dew drops on spider webs is an illustration of how they are one such material capable of efficiently collecting water from air. The water-collecting ability of the capture silk of the Uloborus walckenaerius spider is now shown to be the result of a unique fibre structure that forms after wetting. Many biological surfaces in both the plant and animal kingdom possess unusual structural features at the micro- and nanometre-scale that control their interaction with water and hence wettability 1 , 2 , 3 , 4 , 5 . An intriguing example is provided by desert beetles, which use micrometre-sized patterns of hydrophobic and hydrophilic regions on their backs to capture water from humid air 6 . As anyone who has admired spider webs adorned with dew drops will appreciate, spider silk is also capable of efficiently collecting water from air. Here we show that the water-collecting ability of the capture silk of the cribellate spider Uloborus walckenaerius is the result of a unique fibre structure that forms after wetting, with the ‘wet-rebuilt’ fibres characterized by periodic spindle-knots made of random nanofibrils and separated by joints made of aligned nanofibrils. These structural features result in a surface energy gradient between the spindle-knots and the joints and also in a difference in Laplace pressure, with both factors acting together to achieve continuous condensation and directional collection of water drops around spindle-knots. Submillimetre-sized liquid drops have been driven by surface energy gradients 7 , 8 , 9 or a difference in Laplace pressure 10 , but until now neither force on its own has been used to overcome the larger hysteresis effects that make the movement of micrometre-sized drops more difficult. By tapping into both driving forces, spider silk achieves this task. Inspired by this finding, we designed artificial fibres that mimic the structural features of silk and exhibit its directional water-collecting ability.

The wearable electronic skin with high sensitivity and self-power has shown increasing prospects for applications such as human health monitoring, robotic skin, and intelligent electronic products. In this work, we introduced and demonstrated a design of highly sensitive, self-powered, and wearable electronic skin based on a pressure-sensitive nanofiber woven fabric sensor fabricated by weaving PVDF electrospun yarns of nanofibers coated with PEDOT. Particularly, the nanofiber woven fabric sensor with multi-leveled hierarchical structure, which significantly induced the change in contact area under ultra-low load, showed combined superiority of high sensitivity (18.376 kPa −1 , at ~100 Pa), wide pressure range (0.002–10 kPa), fast response time (15 ms) and better durability (7500 cycles). More importantly, an open-circuit voltage signal of the PPNWF pressure sensor was obtained through applying periodic pressure of 10 kPa, and the output open-circuit voltage exhibited a distinct switching behavior to the applied pressure, indicating the wearable nanofiber woven fabric sensor could be self-powered under an applied pressure. Furthermore, we demonstrated the potential application of this wearable nanofiber woven fabric sensor in electronic skin for health monitoring, human motion detection, and muscle tremor detection.

All-aqueous emulsions exploit spontaneous liquid–liquid separation and due to their water-based nature are particular advantageous for the biocompatible storage and processing of biomacromolecules. However, the ultralow interfacial tensions characteristic of all-aqueous interfaces represent an inherent limitation to the use of thermally adsorbed particles to achieve emulsion stability. Here, we use protein nanofibrils to generate colloidosome-like two-dimensional crosslinked networks of nanostructures templated by all-aqueous emulsions, which we term fibrillosomes. We show that this approach not only allows us to operate below the thermal limit at ultra-low surface tensions but also yields structures that are stable even in the complete absence of an interface. Moreover, we show that the growth and multilayer deposition of fibrils allows us to control the thickness of the capsule shells. These results open up the possibility of stabilizing aqueous two-phase systems using natural proteins, and creating self-standing protein capsules without the requirement for three-phase emulsions or water/oil interfaces. All-aqueous emulsions are useful for delivering and processing biomolecules, but their stability is constrained by low interfacial adsorption energy. Song et al . solve this problem using protein nanofibrils that form a crosslinked network, whose stability is superior to conventional colloidal capsules.

Environmental and health concerns are driving the need for new materials in food packaging to replace poly- or perfluorinated compounds, aluminum layers, and petroleum-based polymers. Cellulose nanofibrils (CNF) have been shown by a number of groups to form excellent barrier layers to oxygen and grease. However, the influence of lignin-containing cellulose nanofibrils (LCNF) on film barrier properties has not been well reported. Herein, thin films (16 g/m2) from LCNF and CNF were formed on paper substrates through a filtration technique that should mimic the addition of material at the wet end of a paper machine. Surface, barrier and mechanical attributes of these samples were characterized. The analysis on the surface free energy and water contact angle pointed to the positive role of lignin distribution in inducing a certain degree of water repellency. The observed oxygen transmission rate (OTR) and water vapor permeability (WVP) values of LCNF-coated samples were nearly similar to those with CNF. However, the presence of lignin improved the oil proof performance; these layered designs exhibited an excellent resistance to grease (kit No. 12). The attained papers with LCNF coat were formed into bowl-like containers using metal molds and a facile oven drying protocol to evaluate their resistance to oil penetration over a longer period. The results confirmed the capability of LCNF layer in holding commercially available cooking oils with no evidence of leakage for over five months. Also, an improvement in the tensile strength and elongation at break was observed in the studied papers. Overall, the proposed packaging material possesses viable architecture and can be considered as a fully wood-based alternative for the current fluorocarbon systems.

Skeletal muscle provides inspiration on how to achieve reversible, macroscopic, anisotropic motion in soft materials. Here we report on the bottom-up design of macroscopic tubes that exhibit anisotropic actuation driven by a thermal stimulus. The tube is built from a hydrogel in which extremely long supramolecular nanofibers are aligned using weak shear forces, followed by radial growth of thermoresponsive polymers from their surfaces. The hierarchically ordered tube exhibits reversible anisotropic actuation with changes in temperature, with much greater contraction perpendicular to the direction of nanofiber alignment. We identify two critical factors for the anisotropic actuation, macroscopic alignment of the supramolecular scaffold and its covalent bonding to polymer chains. Using finite element analysis and molecular calculations, we conclude polymer chain confinement and mechanical reinforcement by rigid supramolecular nanofibers are responsible for the anisotropic actuation. The work reported suggests strategies to create soft active matter with molecularly encoded capacity to perform complex tasks. Skeletal muscles are impressive as they can achieve reversible, macroscopic, anisotropic motion in soft materials. Here the authors show a bottom-up design of macroscopic hydrogel tubes containing supramolecular nanofibers that can undergo anisotropic actuation by thermal stimuli.

Cellulose nanofibril/graphene oxide hybrid (CNF/GO) aerogel was fabricated via a one-step ultrasonication method for adsorptive removal of 21 kinds of antibiotics in water. The as-prepared CNF/GO aerogel possesses interconnected 3D network microstructure, in which GO nanosheets with 2D structure were intimately grown along CNF through hydrogen bonds. The aerogel exhibited superior adsorption capacity toward the antibiotics. The removal percentages (R%) of the antibiotics were more than 69% and the sequence of six categories antibiotics according to the adsorption efficiency was as follows: Tetracyclines > Quinolones > Sulfonamides > Chloramphenicols > β-Lactams > Macrolides. The adsorption mechanism was proposed to be electrostatic attraction, p-π interaction, π-π interaction and hydrogen bonds. In detail, the adsorption capacities of CNF/GO aerogel were 418.7 mg·g −1 for chloramphenicol, 291.8 mg·g −1 for macrolides, 128.3 mg·g −1 for quinolones, 230.7 mg·g −1 for β-Lactams, 227.3 mg·g − 1 for sulfonamides, and 454.6 mg·g −1 for tetracyclines calculated by the Langmuir isotherm models. Furthermore, the regenerated aerogels still could be repeatedly used after ten cycles without obvious degradation of adsorption performance.

One-layer wound dressings cannot meet all the clinical needs due to their individual characteristics and shortcomings. Therefore, bilayer wound dressings which are composed of two layers with different properties have gained lots of attention. In the present study, polycaprolactone/gelatin (PCL/Gel) scaffold was electrospun on a dense membrane composed of polyurethane and ethanolic extract of propolis (PU/EEP). The PU/EEP membrane was used as the top layer to protect the wound area from external contamination and dehydration, while the PCL/Gel scaffold was used as the sublayer to facilitate cells’ adhesion and proliferation. The bilayer wound dressing was investigated regarding its microstructure, mechanical properties, surface wettability, anti-bacterial activity, biodegradability, biocompatibility, and its efficacy in the animal wound model and histopathological analyzes. Scanning electron micrographs exhibited uniform morphology and bead-free structure of the PCL/Gel scaffold with average fibers’ diameter of 237.3 ± 65.1 nm. Significant anti-bacterial activity was observed against Staphylococcal aureus (5.4 ± 0.3 mm), Escherichia coli (1.9 ± 0.4 mm) and Staphylococcus epidermidis (1.0 ± 0.2 mm) according to inhibition zone test. The bilayer wound dressing exhibited high hydrophilicity (51.1 ± 4.9°), biodegradability, and biocompatibility. The bilayer wound dressing could significantly accelerate the wound closure and collagen deposition in the Wistar rats’ skin wound model. Taking together, the PU/EEP-PCL/Gel bilayer wound dressing can be a potential candidate for biomedical applications due to remarkable mechanical properties, biocompatibility, antibacterial features, and wound healing activities.