Ultrastrong and High-Tough Thermoset Epoxy Resins from Hyperbranched Topological Structure and Subnanoscaled Free Volume.

The strength and toughness of thermoset epoxy resins are generally mutually exclusive, as are the high performance and rapid recyclability. Experimentally determined mechanical strength values are usually much lower than their theoretical values. The preparation of thermoset epoxy resins with high modulus, high toughness, ultrastrong strength, and highly efficient recyclability is still a challenge. Here, novel hyperbranched epoxy resins (Bn, n = 6, 12, 24) with imide structures by a thiol-ene click reaction. Bn shows an excellent comprehensive function in simultaneously improving the strength, modulus, toughness, low-temperature resistance, and degradability of diglycidyl ether of bisphenol-A (DGEBA). All the mechanical properties first increase and then decrease with minimization of the free volume properties. The improvement is attributable to uniform molecular holes or free volume by a molecular mixture of linear and hyperbranched topological structures. The precise measurement and controllability of the molecular free volume properties of epoxy resins is first discovered, as well as the imide structure degradation of crosslinked epoxy resins. The two conflicts are successfully resolved between strength and toughness and between high performance during service and high efficiency during degradation. These findings provide a route for designing ultrastrong, tough, and recyclable thermoset epoxy resins.

An efficient interfacial solar evaporator featuring a hierarchical porous structure entirely derived from waste cotton.

Interfacial solar evaporators are widely used to purify water. However, photothermal materials commonly constituting most interfacial solar evaporators remain expensive; additionally, the inherent structure of the evaporators limits their performance. Furthermore, the large amount of waste cotton produced by the textile industry is an environmental threat. To address these issues, we propose an interfacial solar evaporator, H-CA-CS, with a hierarchical porous structure. This evaporator is made entirely of waste cotton and uses carbon microspheres (CMS) and cellulose aerogel (CA) as photothermal and substrate materials, respectively. Additionally, its photothermal layer (CS layer) has large pores and a high porosity, which promote light absorption and timely vapor escape. In contrast, the water transport layer (CA layer) has small pores, providing a robust capillary effect for water transport. Combined with the outstanding light absorption properties of CMS, H-CA-CS exhibited superior overall performance. We found that H-CA-CS has an excellent evaporation rate (1.68 kg m-2 h-1) and an efficiency of 90.6 % under one solar illumination (1 kW m-2), which are superior to those of many waste-based solar evaporators. Moreover, H-CA-CS maintained a mean evaporation rate of 1.61 kg m-2 h-1, ensuring sustainable evaporation performance under long-term scenarios. Additionally, H-CA-CS can be used to purify seawater and various types of wastewater with removal efficiencies exceeding 99 %. In conclusion, this study proposes a method for efficiently using waste cotton to purify water and provides novel ideas for the high-value use of other waste fibers to further mitigate ongoing environmental degradation.

A Lotus Seedpods-Inspired Interfacial Solar Steam Generator with Outstanding Salt Tolerance and Mechanical Properties for Efficient and Stable Seawater Desalination.

Interfacial solar steam generators (ISSGs) can capture solar energy and concentrate the heat at the gas-liquid interface, resulting in efficient water evaporation. However, traditional ISSGs have limitations in long-term seawater desalination processes, such as limited light absorption area, slow water transport speed, severe surface salt accumulation, and weak mechanical performance. Inspired by lotus seedpods, a novel ISSG (rGO-SA-PSF) is developed by treating a 3D warp-knitted spacer fabric with plasma (PSF) and combining it with sodium alginate (SA) and reduces graphene oxide (rGO). The rGO-SA-PSF utilizes a core-suction effect to achieve rapid water pumping and employs aerogel to encapsulate the plasma-treated spacer yarns to create the lotus seedpod-inspired hydrophilic stems, innovatively constructing multiple directional water transport channels. Simultaneously, the large holes of rGO-SA-PSF on the upper layer form lotus seedpod-inspired head concave holes, enabling efficient light capture. Under 1 kW m-2 illumination, rGO-SA-PSF exhibits a rapid evaporation rate of 1.85 kg m-2  h-1 , with an efficiency of 96.4%. Additionally, it shows superior salt tolerance (with no salt accumulation during continuous evaporation for 10 h in 10% brine) and self-desalination performance during long-term seawater desalination processes. This biomimetic ISSG offers a promising solution for efficient and stable seawater desalination and wastewater purification.

A Self-Pumping Dressing with Multiple Liquid Transport Channels for Wound Microclimate Management.

A microclimate with ventilation and proper wettability near the wound is vital for wound healing. In the case of pressure or absorption of large amounts of wound exudate, maintaining air circulation around the wound is currently a challenge for wound dressings. In this study, a novel self-pumping dressing (FAED) with multiple liquid transport channels is designed by combining a 3D spacer fabric, sodium alginate aerogel, and electrospun membrane. This unique structural design allows FAED to unidirectionally rapidly remove excess biofluid from the wound and transfer it through a special liquid transport channel to a liquid storage layer with a high absorption ratio. Importantly, the air circulation layer of FAED composed of liquid transport channels and spacer yarns provides excellent air permeability in both the horizontal (12.3 L min-1 ) and vertical (272.02 mm s-1 ) directions. Additionally, a lower compression modulus (0.14 MPa) and higher compression strength (0.15 MPa) enable the novel dressing to adapt to body contours and provide good supporting performance, as compared to foam dressings. Combined with its high biocompatibility, this unique dressing has significant potential for wound treatment and intensive care.

Closed-Loop Recycling of Both Resin and Fiber from High-Performance Thermoset Epoxy/Carbon Fiber Composites.

Currently, only 5% of thermoset carbon fiber reinforced polymer composites (CFRPs) are recycled into lower-value secondary products. Highly efficient closed-loop recycling of both thermoset resin and carbon fiber is a major challenge. Here, we report a sustainable approach for the closed-loop recycling of the resin and fiber from CFRPs. Thiol-functionalized carbon fiber (TCF) obtained by functionalization with a thiol-ended hyperbranched polymer, and then an epoxy-ended degradable hyperbranched polymer (HT3) are used to prepare HT3/TCF composites, which show considerable acid resistance and mechanical performance. The cured composites are controllably depolymerized into monomers and oligomers with high recyclability (89%), which can be utilized to prepare HT3 and the precursor of cross-linked HT3. A total of 100% of the carbon fibers are recovered and reused to fabricate composites without deterioration of performance. The results provide a method for designing high-performance composites and a pathway for high efficiency closed-loop recycling.

A multifunctional supercapacitor based on 2D nanosheets on a flexible carbon nanotube film.

The manufacture of multifunctional and high-performance wearable supercapacitors (SCs) requires a new class of flexible electrodes with high conductivity, high mechanical stability, good water-proof ability and self-healable capability. Herein, we report a stretchable and self-healable SC based on a MoS2/PEDOT/CNT electrode. The specific capacitance of the SC could be retained up to 81.98% even after the 21st breaking/healing cycle. Furthermore, a sheet-type asymmetric supercapacitor (ASC) based on a MoS2/PEDOT/CNT positive electrode and SnS2/CNT negative electrode is constructed, and it exhibits high performance with an extended potential window of 1.7 V, areal capacitance of 103.76 mF cm-2 at 1.5 mA cm-2, and outstanding stability with no capacitance degradation under a wide range of bending conditions. The ASC is sealed by polyimide films, and it shows high electrochemical stability in hot water and under high speed centrifugation conditions, indicating good water-proof ability and wearability. The as-prepared ASC is also encapsulated in elastic films to provide 225% stretchability. The ASC devices packaged in all these ways exhibit high capacitance retention (>90%) under various bending and dynamic conditions.

Simultaneous Improvement on Strength, Modulus, and Elongation of Carbon Nanotube Films Functionalized by Hyperbranched Polymers.

Carbon nanotube (CNT) buckypapers, or films, have the potential for wide applications because of their unique properties. Neat buckypapers or pristine CNT (PCNT) films have relatively large elongation but low strength and low modulus due to the weak interaction between CNTs. Chemical modifications of PCNT films can significantly strengthen the interaction between CNTs, resulting in high strength and high modulus but usually accompanied by low elongation. Here, we report the functionalization of pristine CNT films by thiol-ended hyperbranched polymers (THBP-n) via a thiol-ene click reaction that can introduce simultaneous improvements on the strength, modulus, and elongation to the PCNT film by 689, 812, and 32.4%, respectively. The high thiol content of THBP-n enables the formation of a network with a high degree of cross-linking between carbon nanotubes, which provides high-efficiency load transfer that increases the tensile strength and modulus of the resulting films and at the same time a compressible hyperbranched structure that allows for deformation and slip between CNTs and consequently improved elongation. The main factors affecting the mechanical performance of the functionalized CNT film are also investigated.

Moisture-Responsive Natural Fiber Coil-Structured Artificial Muscles.

Miniature linear actuators, also known as artificial muscles, mimic the contractile action of skeletal muscles and have potentials in applications, such as soft robotics, prosthetics, exoskeletons, and smart textiles. Natural fibers commonly used in textiles, such as wool, cotton, and flax, are highly anisotropic materials in response to moisture stimulus. Here, we report that this anisotropic property of the natural fibers can be utilized to provide musclelike contractile motions when they are constructed into springlike cylindrical coils by twist insertion. The treatment and conversion of these natural fibers into high-performance musclelike actuators are described. The musclelike actuators made from natural fibers can provide output strain, stress, and work capacity that are orders of magnitude higher than those of animal skeletal muscles and many artificial muscles made from synthetic materials. The natural fiber artificial muscles are demonstrated for potential applications in smart textiles to alleviate body discomfort caused by sweating during sports and other physical activities.

The Dispersion of Pulp-Fiber in High-Density Polyethylene via Different Fabrication Processes.

In this study, a pulp beating machine was used to premix the pulp fibers with high density polyethylene (HDPE) particles in water. The wet or pre-dried pulp fiber/HDPE mixture was then melt-compounded by a twin screw extruder. For further improving the dispersion of pulp fiber, some mixture was forced to pass through the twin-screw extruder twice. The resulting mixture was compression molded to the composite. The fiber distribution was observed by the aid of an optic and scanning electron microscope. The mechanical and rheological properties and creep resistance of the composites were characterized. Test results demonstrate that when the wet pulp fiber/HDPE mixture was subjected to pre-pressing and oven drying prior to extrusion compounding, the resulting composites exhibited homogeneous fiber distribution, superior flexural property, creep-resistance, and high storage modulus. Particularly, its flexural strength and modulus were 57% and 222% higher, respectively, than that of the neat HDPE, while the composites prepared without pre-dried were 19% and 100% higher, respectively. Drying the wet mixture in advance is more effective than re-passing through the extruder for improving the fiber dispersion and composite performance.

Synthesis and Degradation Mechanism of Self-Cured Hyperbranched Epoxy Resins from Natural Citric Acid.

Rapid and highly efficient degradation of cured thermoset epoxy resins is a major challenge to scientists. Here, degradable self-cured hyperbranched epoxy resins (DSHE-n, n = 1, 2, and 3) were synthesized by a reaction between 3-isocyanato-4-methyl-epoxy-methylphenylcarbamate and degradable epoxy-ended hyperbranched polyester (DEHP-n) prepared from maleicanhydride, citric acid, and epichlorohydrin. The chemical structure of DSHE-n was characterized by Fourier transform infrared and 1H NMR spectra. With an increase in DSHE-n molecular weight, the adhesion strength of self-cured DSHE-n films increases distinctly from class 1 to 4, and their pencil hardness remains about class B-2B. The study on the self-cured behavior and mechanism of DSHE-n shows that the carbamate group of the DSHE-n is decomposed into diamine group to react with epoxy group and form a cross-linked structure. The self-cured DSHE-n films were degraded completely in 2 h at 90 °C in the mixed solution of hydrogen peroxide (H2O2) and N,N-dimethylformamide under atmospheric pressure and produced the raw material citric acid, indicating good degradation performance and recyclable property of DSHE-n.

Flexible Asymmetric Threadlike Supercapacitors Based on NiCo2 Se4 Nanosheet and NiCo2 O4 /Polypyrrole Electrodes.

Flexible threadlike supercapacitors with improved performance are needed for many wearable electronics applications. Here, we report a high performance flexible asymmetric all-solid-state threadlike supercapacitor with a NiCo2 Se4 positive electrode and a NiCo2 O4 @PPy (PPy: polypyrrole) negative electrode. The as-prepared electrodes display outstanding volume specific capacitance (14.2 F cm-3 ) and excellent cycling performance (94 % retention after 5000 cycles at 0.6 mA) owing to their nanosheet and nanosphere structures. The asymmetric all-solid-state threadlike supercapacitor expanded the stability voltage window from 0-1.0 V to 0-1.7 V and exhibits high volume energy density (5.18 mWh cm-3 ) and superior flexibility under different bending conditions. This study provides a scalable method for fabricating high performance flexible supercapacitors from easily available materials for use in wearable and portable electronics.

Synthesis of a Degradable High-Performance Epoxy-Ended Hyperbranched Polyester.

Degradation and recycling of cured thermosetting epoxy resins are major challenges to the industry. Here, a low-viscosity, degradable epoxy-ended hyperbranched polyester (DEHP) is synthesized by a reaction between epichlorohydrin and a carboxyl-ended hyperbranched polyester (DCHP) obtained from an esterification between citric acid and maleic anhydride. The chemical structures of DCHP and DEHP were characterized by Fourier transform infrared and 1H NMR. DEHP has a positive effect on reinforcing and toughening of the diglycidyl ether of bisphenol-A (DGEBA). With an increase in the content and molecular weight of DEHP, the mechanical performances of the cured DEHP/DGEBA composites, including the tensile, flexural, and impact strengths, increase first and then decrease. The improvements on the tensile, flexural, and impact strengths were 34.2-43.4%, 35.6-48.1%, and 117.9-137.8%, respectively. Moreover, the DEHP also promotes degradation of the cured DEHP/DGEBA composites. The degree of degradation of the cured DEHP/DGEBA composites increases with an increase of the DEHP content and molecular weight. The composites containing 12 wt % DEHP can be degraded completely in only about 2 h at about 90 °C, compared with the degradation degree (35%) of cured DGEBA, indicating good degradation and recycling properties of the DEHP.

High Performance Carbon Nanotube Yarn Supercapacitors with a Surface-Oxidized Copper Current Collector.

Threadlike linear supercapacitors have demonstrated high potential for constructing fabrics to power electronic textiles (eTextiles). To improve the cyclic electrochemical performance and to produce power fabrics large enough for practical applications, a current collector has been introduced into the linear supercapcitors to transport charges produced by active materials along the length of the supercapacitor with high efficiency. Here, we first screened six candidate metal filaments (Pt, Au, Ag, AuAg, PtCu, and Cu) as current collectors for carbon nanotube (CNT) yarn-based linear supercapacitors. Although all of the metal filaments significantly improved the electrochemical performance of the linear supercapacitor, two supercapacitors constructed from Cu and PtCu filaments, respectively, demonstrate far better electrochemical performance than the other four supercapacitors. Further investigation shows that the surfaces of the two Cu-containing filaments are oxidized by the surrounding polymer electrolyte in the electrode. While the unoxidized core of the Cu-containing filaments remains highly conductive and functions as a current collector, the resulting CuO on the surface is an electrochemically active material. The linear supercapacitor architecture incorporating dual active materials CNT + Cu extends the potential window from 1.0 to 1.4 V, leading to significant improvement to the energy density and power density.

High-performance two-ply yarn supercapacitors based on carbon nanotube yarns dotted with Co3 O4 and NiO nanoparticles.

Yarn supercapacitors are promising power sources for flexible electronic applications that require conventional fabric-like durability and wearer comfort. Carbon nanotube (CNT) yarn is an attractive choice for constructing yarn supercapacitors used in wearable textiles because of its high strength and flexibility. However, low capacitance and energy density limits the use of pure CNT yarn in wearable high-energy density devices. Here, transitional metal oxide pseudocapacitive materials NiO and Co3 O4 are deposited on as-spun CNT yarn surface using a simple electrodeposition process. The Co3 O4 deposited on the CNT yarn surface forms a uniform hybridized CNT@Co3 O4 layer. The two-ply supercapacitors formed from the CNT@Co3 O4 composite yarns display excellent electrochemical properties with very high capacitance of 52.6 mF cm(-2) and energy density of 1.10 µWh cm(-2) . The high performance two-ply CNT@Co3 O4 yarn supercapacitors are mechanically and electrochemically robust to meet the high performance requirements of power sources for wearable electronics.

Self-assembly of amido-ended hyperbranched polyester films with a highly ordered dendritic structure.

Self-assemblies fabricated from dendrimers and amphiphilic polymers have demonstrated remarkable performances and a wide range of applications. Direct self-assembly of hyperbranched polymers into highly ordered macrostructures with heat-resistance remains a big challenge due to the weak amphiphilicity of the polymers. Here, we report the self-assembly of amphiphilic amido-ended hyperbranched polyester (HTDA-2) into millimeter-size dendritic films using combined hydrogen bond interaction and solvent induction. The self-assembly process and mechanism have been studied. Hydrogen bond interaction between amido-ended groups assists the aggregation of inner and outer chains of the HTDA-2, resulting in phase separation and micelle formation. Some micelles attach to and grow on the glass substrate like seedlings. Other micelles move to the seedlings and connect with their branches via solvent induction and hydrogen bond interaction, leading to the fabrication of highly ordered crystalline dendritic films that show high heat-resistance. HTDA-2 can further self-assemble into sheet crystals on the dendritic films.

Metallic conductivity transition of carbon nanotube yarns coated with silver particles.

Dry spun carbon nanotube yarns made from vertically aligned multiwalled carbon nanotube forests possess high mechanical strength and behave like semiconductors with electrical conductivity of the order of 4 × 10(4) S m(-1). Coating a submicron-thick film of silver particle-filled polymer on the surface increased the electrical conductivity of the carbon nanotube yarn by 60-fold without significantly sacrificing its mechanical strength. The transitional characteristics of the silver-coated carbon nanotube yarn were investigated by varying the take-up ratio of the silver coating. A step change in conductivity was observed when the silver content in the coated yarn was between 7 and 10 wt% as a result of the formation of connected silver particle networks on the carbon nanotube yarn surface.

Core-spun carbon nanotube yarn supercapacitors for wearable electronic textiles.

Linear (fiber or yarn) supercapacitors have demonstrated remarkable cyclic electrochemical performance as power source for wearable electronic textiles. The challenges are, first, to scale up the linear supercapacitors to a length that is suitable for textile manufacturing while their electrochemical performance is maintained or preferably further improved and, second, to develop practical, continuous production technology for these linear supercapacitors. Here, we present a core/sheath structured carbon nanotube yarn architecture and a method for one-step continuous spinning of the core/sheath yarn that can be made into long linear supercapacitors. In the core/sheath structured yarn, the carbon nanotubes form a thin surface layer around a highly conductive metal filament core, which serves as current collector so that charges produced on the active materials along the length of the supercapacitor are transported efficiently, resulting in significant improvement in electrochemical performance and scale up of the supercapacitor length. The long, strong, and flexible threadlike supercapacitor is suitable for production of large-size fabrics for wearable electronic applications.

Asymmetric carbon nanotube-MnO2 two-ply yarn supercapacitors for wearable electronics.

Strong and flexible two-ply carbon nanotube yarn supercapacitors are electrical double layer capacitors that possess relatively low energy storage capacity. Pseudocapacitance metal oxides such as MnO2 are well known for their high electrochemical performance and can be coated on carbon nanotube yarns to significantly improve the performance of two-ply carbon nanotube yarn supercapacitors. We produced a high performance asymmetric two-ply yarn supercapacitor from as-spun CNT yarn and CNT@Mn22 composite yarn in aqueous electrolyte. The as-spun CNT yarn serves as negative electrode and the CNT@MnO2 composite yarn as positive electrode. This asymmetric architecture allows the operating potential window to be extended from 1.0 to 2.0 V and results in much higher energy and power densities than the reference symmetric two-ply yarn supercapacitors, reaching 42.0 Wh kg(-1) at a lower power density of 483.7 W kg(-1), and 28.02 Wh kg(-1) at a higher power density of 19,250 W kg(-1). The asymmetric supercapacitor can sustain cyclic charge-discharge and repeated folding/unfolding actions without suffering significant deterioration of specific capacitance. The combination of high strength, flexibility and electrochemical performance makes the asymmetric two-ply yarn supercapacitor a suitable power source for flexible electronic devices for applications that require high durability and wearer comfort.

Gamma-irradiated carbon nanotube yarn as substrate for high-performance fiber supercapacitors.

As an electrical double layer capacitor, dry-spun carbon nanotube yarn possesses relatively low specific capacitance. This can be significantly increased as a result of the pseudocapacitance of functional groups on the carbon nanotubes developed by oxidation using a gamma irradiation treatment in the presence of air. When coated with high-performance polyaniline nanowires, the gamma-irradiated carbon nanotube yarn acts as a high-strength reinforcement and a high-efficiency current collector in two-ply yarn supercapacitors for transporting charges generated along the long electrodes. The resulting supercapacitors demonstrate excellent electrochemical performance, cycle stability, and resistance to folding-unfolding that are required in wearable electronic textiles.

High-performance two-ply yarn supercapacitors based on carbon nanotubes and polyaniline nanowire arrays.

Fine count two-ply yarn supercapacitors are constructed from carbon nanotube yarns and polyaniline nanowires. The thread-like supercapacitor possess excellent electrochemical capacity and are very strong and flexible. When being woven or knitted into wearable electronic devices, alone or in combination with conventional textile yarns, the two-ply yarn supercapacitors can be flexed and stretched repeatedly without significant loss of capacitance.