One‐Step Wet‐Spinning Process of Poly(3,4‐ethylenedioxythiophene):Poly(styrenesulfonate) Fibers and the Origin of Higher Electrical Conductivity

A simplified wet‐spinning process for the production of continuous poly (3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) fibers is reported. Conductivity enhancement of PEDOT:PSS fibers up to 223 S cm^?1 has been demonstrated when these fibers are exposed to ethylene glycol as a post‐synthesis processing step. In a new spinning approach it is shown that by employing a spinning formulation consisting of an aqueous blend of PEDOT:PSS and poly(ethlylene glycol), the need for post‐spinning treatment with ethylene glycol is eliminated. With this approach, 30‐fold conductivity enhancements from 9 to 264 S cm^?1 are achieved with respect to an untreated fiber. This one‐step approach also demonstrates a significant enhancement in the redox properties of the fibers. These improvements are attributed to an improved molecular ordering of the PEDOT chains in the direction of the fiber axis and the consequential enrichment of linear (or expanded‐coil like) conformation to preference bipolaronic electronic structures as evidenced by Raman spectroscopy, solid‐state electron spin resonance (ESR) and in situ electrochemical ESR studies.     

Arbitrarily Shaped Fiber Assemblies from Spun Carbon Nanotube Gel Fibers

Experimental methods, apparatus, and practically useful theoretical analysis are provided for the coagulation‐based spinning of effectively unlimited lengths of carbon nanotube fibers having exceptional toughness and reasonably high strength. This spinning process fundamentally depends on the mechanical properties of intermediate gel state fibers, which we find are surprising elastic up to about 20 % strain and sufficiently strong for diverse processing methods. More specifically, we show that assemblies of these gel fibers can be used as intermediates for making nanotube sheets, large diameter fibers, and conformal coatings. When suitably processed, these composites (comprising many parallel solution‐spun nanotube fibers) have useful strength and extraordinary toughness.     

Lightweight and Anisotropic Porous MWCNT/WPU Composites for Ultrahigh Performance Electromagnetic Interference Shielding

Lightweight, flexible and anisotropic porous multiwalled carbon nanotube (MWCNT)/water‐borne polyurethane (WPU) composites are assembled by a facile freeze‐drying method. The composites contain extremely wide range of MWCNT mass ratios and show giant electromagnetic interference (EMI) shielding effectiveness (SE) which exceeds 50 or 20 dB in the X‐band while the density is merely 126 or 20 mg cm^?3, respectively. The relevant specific SE is up to 1148 dB cm³ g^?1, greater than those of other shielding materials ever reported. The ultrahigh EMI shielding performance is attributed to the conductivity of the cell walls caused by MWCNT content, the anisotropic porous structures, and the polarization between MWCNT and WPU matrix. In addition to the enhanced electrical properties, the composites also indicate enhanced mechanical properties compared with porous WPU and CNT architectures.     

Ambient‐Dried Cellulose Nanofibril Aerogel Membranes with High Tensile Strength and Their Use for Aerosol Collection and Templates for Transparent,Flexible Devices

The application potential of cellulose nanofibril (CNF) aerogels has been hindered by the slow and costly freeze‐ or supercritical drying methods. Here, CNF aerogel membranes with attractive mechanical, optical, and gas transport properties are prepared in ambient conditions with a facile and scalable process. Aqueous CNF dispersions are vacuum‐filtered and solvent exchanged to 2‐propanol and further to octane, followed by ambient drying. The resulting CNF aerogel membranes are characterized by high transparency (>90% transmittance), stiffness (6 GPa Young's modulus, 10 GPa cm³ g^?1 specific modulus), strength (97 MPa tensile strength, 161 MPa m³ kg^?1 specific strength), mesoporosity (pore diameter 10–30 nm, 208 m² g^?1 specific surface area), and low density (≈0.6 g cm^?3). They are gas permeable thus enabling collection of nanoparticles (for example, single‐walled carbon nanotubes, SWNT) from aerosols under pressure gradients. The membranes with deposited SWNT can be further compacted to transparent, conductive, and flexible conducting films (90% specular transmittance at 550 nm and 300 Ω ?^{? 1} sheet resistance with AuCl₃‐salt doping). Overall, the developed aerogel membranes pave way toward use in gas filtration and transparent, flexible devices.     

Properties of Carbon Nanotube Fibers Spun from DNA‐Stabilized Dispersions

The fabrication of single‐walled carbon nanotube (CNT) fibers containing (salmon) DNA has been demonstrated. The DNA material has been found to be adequate for dispersing relatively large concentrations (up to 1 % by weight) of carbon nanotubes. These dispersions are better suited for fiber spinning than previously studied dispersions based on conventional surfactants, such as sodium dodecyl sulfate (SDS). The DNA‐containing fibers were less conductive than the fibers based on SDS, but they were significantly stronger. Considerably increased conductivity was obtained by thermally annealing the CNT/DNA fibers, a process accompanied by a loss in mechanical strength. Smaller improvements in conductivity could be introduced by annealing the carbon nanotubes before fiber production, with no alteration of the fiber mechanical properties. Those CNT/DNA fibers that were mechanically strong and conductive also exhibited good electrochemical behavior and useful capacitance values (up to 7.2 F g^–1).     

Elasticity,Flexibility, and Ideal Strength of Borophenes

The mechanical properties of 2D boron—borophene—are studied by first‐principles calculations. The recently synthesized borophene with a 1/6 concentration of hollow hexagons (HH) is shown to have in‐plane modulus C up to 210 N m^?1 and bending stiffness as low as D = 0.39 eV. Thus, its Foppl–von Karman number per unit area, defined as C /D , reaches 568 nm^?2, over twofold higher than graphene's value, establishing the borophene as one of the most flexible materials. Yet, the borophene has a specific modulus of 346 m² s^?2 and ideal strength of 16 N m^?1, rivaling those (453 m² s^?2 and 34 N m^?1) of graphene. In particular, its structural fluxionality enabled by delocalized multicenter chemical bonding favors structural phase transitions under tension, which result in exceptionally small breaking strains yet highly ductile breaking behavior. These mechanical properties can be further tailored by varying the HH concentration, and the boron sheet without HHs can even be stiffer than graphene against tension. The record high flexibility combined with excellent elasticity in boron sheets can be utilized for designing advanced composites and flexible devices.     

High Strength Conductive Composites with Plasmonic Nanoparticles Aligned on Aramid Nanofibers

Rapidly evolving fields of biomedical, energy, and (opto)electronic devices bring forward the need for deformable conductors with constantly rising benchmarks for mechanical properties and electronic conductivity. The search for conductors with improved strength and strain have inspired the multiple studies of nanocomposites and amorphous metals. However, finding conductors that defy the boundaries of classical materials and exhibit simultaneously high strength, toughness, and fast charge transport while enabling their scalable production, remains a difficult materials engineering challenge. Here, composites made from aramid nanofibers (ANFs) and gold nanoparticles (Au NPs) that offer a new toolset for engineering high strength flexible conductors are described. ANFs are derived from Kevlar macrofibers and retain their strong mechanical properties and temperature resilience. Au NPs are infiltrated into a porous, free‐standing aramid matrix, becoming aligned on ANFs, which reduces the charge percolation threshold and facilitates charge transport. Further thermal annealing at 300 °C results in the Au‐ANF composites with an electrical conductivity of 1.25 × 10⁴ S cm^?1 combined with a tensile strength of 96 MPa, a Young's modulus of 5.29 GPa, and a toughness of 1.3 MJ m^?3. These parameters exceed those of most of the composite materials, and are comparable to those of amorphous metals but have no volume limitations. The plasmonic optical frequencies characteristic for constituent NPs are present in the composites with ANFs enabling plasmon‐based optoelectronic applications.     

Strain‐Responsive Polyurethane/PEDOT:PSS Elastomeric Composite Fibers with High Electrical Conductivity

It is a challenge to retain the high stretchability of an elastomer when used in polymer composites. Likewise, the high conductivity of organic conductors is typically compromised when used as filler in composite systems. Here, it is possible to achieve elastomeric fiber composites with high electrical conductivity at relatively low loading of the conductor and, more importantly, to attain mechanical properties that are useful in strain‐sensing applications. The preparation of homogenous composite formulations from poly­urethane (PU) and poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) that are also processable by fiber wet‐spinning techniques are systematically evaluated. With increasing PEDOT:PSS loading in the fiber composites, the Young's modulus increases exponentially and the yield stress increases linearly. A model describing the effects of the reversible and irreversible deformations as a result of the re‐arrangement of PEDOT:PSS filler networks within PU and how this relates to the electromechanical properties of the fibers during the tensile and cyclic stretching is presented.     

High Mechanical Performance Composite Conductor: Multi‐Walled Carbon Nanotube Sheet/Bismaleimide Nanocomposites

Multi‐walled carbon nanotube (MWNT)‐sheet‐reinforced bismaleimide (BMI) resin nanocomposites with high concentrations (～60 wt%) of aligned MWNTs are successfully fabricated. Applying simple mechanical stretching and prepregging (pre‐resin impregnation) processes on initially randomly dispersed, commercially available sheets of millimeter‐long MWNTs leads to substantial alignment enhancement, good dispersion, and high packing density of nanotubes in the resultant nanocomposites. The tensile strength and Young's modulus of the nanocomposites reaches 2 088 MPa and 169 GPa, respectively, which are very high experimental results and comparable to the state‐of‐the‐art unidirectional IM7 carbon‐fiber‐reinforced composites for high‐performance structural applications. The nanocomposites demonstrate unprecedentedly high electrical conductivity of 5 500 S cm^?1 along the alignment direction. Such unique integration of high mechanical properties and electrical conductance opens the door for developing polymeric composite conductors and eventually structural composites with multifunctionalities. New fracture morphology and failure modes due to self‐assembly and spreading of MWNT bundles are also observed.     

Clay Assisted Dispersion of Carbon Nanotubes in Conductive Epoxy Nanocomposites

Clay was introduced into single‐walled carbon nanotube (SWNT)/epoxy composites to improve nanotube dispersion without harming electrical conductivity or mechanical performance. Unlike surfactant or polymer dispersants, clay is mechanically rigid and known to enhance the properties (e.g., modulus, gas barrier, and flame retardation) of polymer composites. Combining nanotubes and clay allows both electrical and mechanical behavior to be simultaneously enhanced. With just 0.05 wt % SWNT, electrical conductivity is increased by more than four orders of magnitude (from 10^–9 to 10^–5 S cm^–1) with the addition of 0.2 wt % clay. Furthermore, the percolation threshold of these nanocomposites is reduced from 0.05 wt % SWNT to 0.01 wt % with the addition of clay. SWNTs appear to have an affinity for clay that causes them to become more exfoliated and better networked in these composites. This clay‐nanotube synergy may make these composites better suited for a variety of packaging, sensing, and shielding applications.     

Lithium–Sulfur Battery Cable Made from Ultralight,Flexible Graphene/Carbon Nanotube/Sulfur Composite Fibers

The emergence of flexible and wearable electronic devices with shape amenability and high mobility has stimulated the development of flexible power sources to bring revolutionary changes to daily lives. The conventional rechargeable batteries with fixed geometries and sizes have limited their functionalities in wearable applications. The first‐ever graphene‐based fibrous rechargeable batteries are reported in this work. Ultralight composite fibers consisting of reduced graphene oxide/carbon nanotube filled with a large amount of sulfur (rGO/CNT/S) are prepared by a facile, one‐pot wet‐spinning method. The liquid crystalline behavior of high concentration GO sheets facilitates the alignment of rGO/CNT/S composites, enabling rational assembly into flexible and conductive fibers as lithium–sulfur battery electrodes. The ultralight fiber electrodes with scalable linear densities ranging from 0.028 to 0.13 mg cm^?1 deliver a high initial capacity of 1255 mAh g^?1 and an areal capacity of 2.49 mAh cm^?2 at C /20. A shape‐conformable cable battery prototype demonstrates a stable discharge characteristic after 30 bending cycles.     

Flexible Thermoelectric Polymer Composites Based on a Carbon Nanotubes Forest

Polymer‐based composites are of high interest in the field of thermoelectric (TE) materials because of their properties: abundance, low thermal conductivity, and nontoxicity. In applications, like TE for wearable energy harvesting, where low operating temperatures are required, polymer composites demonstrate compatible with the targeted specifications. The main challenge is reaching high TE efficiency. Fillers and chemical treatments can be used to enhance TE performance of the polymer matrix. The combined application of vertically aligned carbon nanotubes forest (VA‐CNTF) is demonstrated as fillers and chemical post‐treatment to obtain high‐efficiency TE composites, by dispersing VA‐CNTF into a poly (3,4‐ethylenedioxythiophene) polystyrene sulfonate matrix. The VA‐CNTF keeps the functional properties even in flexible substrates. The morphology, structure, composition, and functional features of the composites are thoroughly investigated. A dramatic increase of power factor is observed at the lowest operating temperature difference ever reported. The highest Seebeck coefficient and electrical conductivity are 58.7 µV K^?1 and 1131 S cm^?1, respectively. The highest power factor after treatment is twice as high in untreated samples. The results demonstrate the potential for the combined application of VA‐CNTF and chemical post‐treatment, in boosting the TE properties of composite polymers toward the development of high efficiency, low‐temperature, flexible TEs.     

High‐Yield Fabrication,Activation, and Characterization of Carbon Nanotube Ion Channels by Repeated Voltage‐Ramping of Membrane‐Capillary Assembly

The interior channels of carbon nanotubes are promising for studying transport of individual molecules in a 1D confined space. However, experimental investigations of the interior transport have been limited by the extremely low yields of fabricated nanochannels and their characterization. Here, this challenge is addressed by assembling nanotube membranes on glass capillaries and employing a voltage‐ramping protocol. Centimeter‐long carbon nanotubes embedded in an epoxy matrix are sliced to hundreds of 10 µm‐thick membranes containing essentially identical nanotubes. The membrane is attached to glass capillaries and dipped into analyte solution. Repeated ramping of the transmembrane voltage gradually increases ion conductance and activates the nanotube ion channels in 90% of the membranes; 33% of the activated membranes exhibit stochastic pore‐blocking events caused by cation translocation through the interiors of the nanotubes. Since the membrane‐capillary assembly can be handled independently of the analyte solution, fluidic exchange can be carried out simply by dipping the capillary into a solution of another analyte. This capability is demonstrated by sequentially measuring the threshold transmembrane voltages and ion mobilities for K⁺, Na⁺, and Li⁺. This approach, validated with carbon nanotubes, will save significant time and effort when preparing and testing a broad range of solid‐state nanopores.     

Carbon‐Nanotube‐Reinforced Zr‐Based Bulk Metallic Glass Composites and Their Properties

In this paper, we systematically report the preparation of carbon‐nanotube (CNT)‐reinforced Zr‐based bulk metallic glass (BMG) composites. The physical and mechanical properties of the composites were investigated. Compressive testing shows that the composites still display high fracture strength. Investigation also shows that the composites have strong ultrasonic attenuation characteristics and excellent wave absorption ability. The strong wave absorption implies that CNT‐reinforced Zr‐based BMG composites, besides their excellent mechanical properties, may also have significant potential for applications in shielding acoustic sound or environmental noise.     

Aramid Nanofiber Membranes for Energy Harvesting from Proton Gradients

Harvesting osmotic energy from industrial wastewater is an often-overlooked source of electricity that can be used as a part of the comprehensive distributed energy systems. However, this concept requires, a new generation of inexpensive ion-selective membranes that must withstand harsh chemical conditions with both high/low pH, have high temperature resilience, display exceptional mechanical properties, and support high ionic conductance. Here, aramid nanofibers (ANFs) based membranes with high chemical/thermal stability, mechanical strength, toughness, and surface charge density make them capable of high-performance osmotic energy harvesting from pH gradients generated upon wastewater dilution. ANF membranes produce an averaged output power density of 17.3 W m^?2 for more than 240 h at pH 0. Taking advantage of the high temperature resilience of aramid, the output power density is increased further to 77 W m^?2 at 70 °C, typical for industrial wastewater. Such output power performance is 10× better compared to the current state-of-the-art membranes being augmented by Kevlar-like environmental robustness of ANF membranes. The improved efficiency of energy harvesting is ascribed to the high proton selectivity of ANFs. Retaining high output power density for large membrane area and fluoride-free synthesis of ANFs from recyclable material opens the door for scalable wastewater energy harvesting.     

Programmable Liquid Metal Microstructures for Multifunctional Soft Thermal Composites

Soft, elastically deformable composites can enable new generations of multifunctional materials for electronics, robotics, and reconfigurable structures. Liquid metal (LM) droplets dispersed in elastomer matrices represent an emerging material architecture that has shown unique combinations of soft mechanical response with exceptional electrical and thermal functionalities. These properties are strongly dependent on the material composition and microstructure. However, approaches to control LM microdroplet morphology to program mechanical and functional properties are lacking. Here, this limitation is overcome by thermo‐mechanically shaping LM droplets in soft composites to create programmable microstructures in stress‐free materials. This enables LM loadings up to 70% by volume with prescribed particle aspect ratios and orientation, enabling control of microstructure throughout the bulk of the material. Through this microstructural control in soft composites, a material which simultaneously achieves a thermal conductivity as high as 13.0 W m^?1 K^?1 (>70 × increase over polymer matrix) with low modulus (<1.0 MPa) and high stretchability (>750% strain) is demonstrated in stress‐free conditions. Such properties are required in applications that demand extreme mechanical flexibility with high thermal conductivity, which is demonstrated in soft electronics, wearable robotics, and electronics integrated into 3D printed materials.     

Chemically Resistant,Shapeable, and Conducting Metal‐Organic Gels and Aerogels Built from Dithiooxamidato Ligand

Metal‐organic gels (MOGs) appear as a blooming alternative to well‐known metal‐organic frameworks (MOFs). Porosity of MOGs has a microstructural origin and not strictly crystalline like in MOFs; therefore, gelation may provide porosity to any metal‐organic system, including those with interesting properties but without a porous crystalline structure. The easy and straightforward shaping of MOGs contrasts with the need of binders for MOFs. In this contribution, a series of MOGs based on the assembly of 1D‐coordination polymer nanofibers of formula [M(DTA)]_n (M^II: Ni, Cu, Pd; DTA: dithiooxamidato) are reported, in which properties such as porosity, chemical inertness, mechanical robustness, and stimuli‐responsive electrical conductivity are brought together. The strength of the M? S bond confers an unusual chemical resistance, withstanding exposure to acids, alkalis, and mild oxidizing/reducing chemicals. Supercritical drying of MOGs provides ultralight metal‐organic aerogels (MOAs) with densities as low as 0.03 g cm^?3 and plastic/brittle behavior depending on the nanofiber aspect ratio. Conductivity measurements reveal a semiconducting behavior (10^?12 to 10^?7 S cm^?1 at 298 K) that can be improved by doping (10^?5 S cm^?1). Moreover, it must be stressed that conductivity of MOAs reversibly increases (up to 10^?5 S cm^?1) under the presence of acetic acid.     

Scaling the Stiffness,Strength, and Toughness of Ceramic‐Coated Nanotube Foams into the Structural Regime

Natural materials such as bone and tooth achieve precisely tuned mechanical and interfacial properties by varying the concentration and orientation of their nanoscale constituents. However, the realization of such control in engineered foams is limited by manufacturing‐driven tradeoffs among the size, order, and dispersion uniformity of the building blocks. It is demonstrated how to manufacture nanocomposite foams with precisely controllable mechanical properties via aligned carbon nanotube (CNT) growth followed by atomic layer deposition (ALD). By starting with a low density CNT forest and varying the ALD coating thickness, we realize predictable ≈1000‐fold control of Young's modulus (14 MPa to 20 GPa, where E ～ ρ ^2.8), ultimate compressive strength (0.8 MPa to 0.16 GPa), and energy absorption (0.4 to 400 J cm^–3). Owing to the continuous, long CNTs within the ceramic nanocomposite, the compressive strength and toughness of the new material are 10‐fold greater than commercially available aluminum foam over the same density range. Moreover, the compressive stiffness and strength equal that of compact bone at 10% lower density. Along with emerging technologies for scalable patterning and roll‐to‐roll manufacturing and lamination of CNT films, coated CNT foams may be especially suited to multifunctional applications such as catalysis, filtration, and thermal protection.     

One‐Pot Synthesis of Antimony‐Embedded Silicon Oxycarbide Materials for High‐Performance Sodium‐Ion Batteries

Sodium‐ion batteries have recently attracted intensive attention due to their natural abundance and low cost. Antimony is a desirable candidate for an anode material for sodium‐ion batteries due to its high theoretical capacity (660 mA h g^?1). However, the utilization of alloy‐based anodes is still limited by their inherent huge volume changes and sluggish kinetics. The Sb‐embedded silicon oxycarbide (SiOC) composites are simply synthesized via a one‐pot pyrolysis process at 900 °C without any additives or surfactants, taking advantage of the superior self‐dispersion properties of antimony acetate powders in silicone oil. The structural and morphological characterizations confirm that Sb nanoparticles are homogeneously embedded into the amorphous SiOC matrix. The composite materials exhibit an initial desodiation capacity of around 510 mA h g^?1 and maintained an excellent capacity retention above 97% after 250 cycles. The rate capability test reveals that the composites deliver capacity greater than 453 mA h g^?1, even at the high current density of 20 C rate, owing to the free‐carbon domain of SiOC material. The electrochemical and postmortem analyses confirm that the SiOC matrix with a uniform distribution of Sb nanoparticles provides the mechanical strength without degradation in conductive characteristics, suppressing the agglomeration of Sb particles during the electrochemical reaction.     

Reinforcing Epoxy Polymer Composites Through Covalent Integration of Functionalized Nanotubes

Strong interfacial bonding and homogenous dispersion have been found to be necessary conditions to take full advantage of the extraordinary properties of nanotubes for reinforcement of composites. We have developed a fully integrated nanotube composite material through the use of functionalized single‐walled carbon nanotubes (SWNTs). The functionalization was performed via the reaction of terminal diamines with alkylcarboxyl groups attached to the SWNTs in the course of a dicarboxylic acid acyl peroxide treatment. Nanotube‐reinforced epoxy polymer composites were prepared by dissolving the functionalized SWNTs in organic solvent followed by mixing with epoxy resin and curing agent. In this hybrid material system, nanotubes are covalently integrated into the epoxy matrix and become part of the crosslinked structure rather than just a separate component. Results demonstrated dramatic enhancement in the mechanical properties of an epoxy polymer material, for example, 30–70 % increase in ultimate strength and modulus with the addition of only small quantities (1–4 wt.‐%) of functionalized SWNTs. The nanotube‐reinforced epoxy composites also exhibited an increased strain to failure, which suggests higher toughness.