Knittable Electrochemical Yarn Muscle for Morphing Textiles.

Morphing textiles, crafted using electrochemical artificial muscle yarns, boast features such as adaptive structural flexibility, programmable control, low operating voltage, and minimal thermal effect. However, the progression of these textiles is still impeded by the challenges in the continuous production of these yarn muscles and the necessity for proper structure designs that bypass operation in extensive electrolyte environments. Herein, a meters-long sheath-core structured carbon nanotube (CNT)/nylon composite yarn muscle is continuously prepared. The nylon core not only reduces the consumption of CNTs but also amplifies the surface area for interaction between the CNT yarn and the electrolyte, leading to an enhanced effective actuation volume. When driven electrochemically, the CNT@nylon yarn muscle demonstrates a maximum contractile stroke of 26.4%, a maximum contractile rate of 15.8% s-1, and a maximum power density of 0.37 W g-1, surpassing pure CNT yarn muscles by 1.59, 1.82, and 5.5 times, respectively. By knitting the electrochemical CNT@nylon artificial muscle yarns into a soft fabric that serves as both a soft scaffold and an electrolyte container, we achieved a morphing textile is achieved. This textile can perform programmable multiple motion modes in air such as contraction and sectional bending.

Construction of Medusa-Like Adhesive Carbon Nanotube Array Induced by Deformation of Alumina Sheets.

To change the binary structure of nanotube and nanotube array in vertically aligned carbon nanotube arrays, this work deposits regularly arranged amorphous alumina sheets on the classical array growth catalyst (10 nm-thick alumina and 2 nm-thick iron) and obtains an array similar to the Medusa head. Subsequent experiments revealed that these alumina sheets show both unstable and stable qualities during growth: unstable in that they thermally deform and change their newly discovered characteristics of blocking carbon source diffusion, which regulates the nanotube growth order in specific areas; stable in that they withstand the deformation caused by heat and sequential growth of nanotubes, serving as a substrate and buffer layer for Medusa's hair, i.e., nanotube bundles on the array surface. Their combination splits this binary structure into a tertiary architecture consisting of nanotubes, nanotube bundles, and the array spanning nano-, micro-, and milli-meter. Benefiting from this structure, this array exhibits a unique near-isotropic adhesion characteristic compared to existing reports and outperforms classical and patterned arrays with the same classical catalyst and growth conditions.

Direct recycling of spent Li-ion batteries: Challenges and opportunities toward practical applications.

With the exponential expansion of electric vehicles (EVs), the disposal of Li-ion batteries (LIBs) is poised to increase significantly in the coming years. Effective recycling of these batteries is essential to address environmental concerns and tap into their economic value. Direct recycling has recently emerged as a promising solution at the laboratory level, offering significant environmental benefits and economic viability compared to pyrometallurgical and hydrometallurgical recycling methods. However, its commercialization has not been realized in the terms of financial feasibility. This perspective provides a comprehensive analysis of the obstacles that impede the practical implementation of direct recycling, ranging from disassembling, sorting, and separation to technological limitations. Furthermore, potential solutions are suggested to tackle these challenges in the short term. The need for long-term, collaborative endeavors among manufacturers, battery producers, and recycling companies is outlined to advance fully automated recycling of spent LIBs. Lastly, a smart direct recycling framework is proposed to achieve the full life cycle sustainability of LIBs.

Direct Regeneration of NCM Cathode Material with Aluminum Scraps.

Hydrothermal-based direct regeneration of spent Li-ion battery (LIB) cathodes has garnered tremendous attention for its simplicity and scalability. However, it is heavily reliant on manual disassembly to ensure the high purity of degraded cathode powders, and the quality of regenerated materials. In reality, degraded cathodes often contain residual components of the battery, such as binders, current collectors, and graphite particles. Thorough investigation is thus required to understand the effects of these impurities on hydrothermal-based direct regeneration. In this study, we focus on isolating the effects of aluminum (Al) scraps on the direct regeneration process. We found that Al metal can be dissolved during the hydrothermal relithiation process. Even when the cathode material contains up to 15 wt.% Al scraps, no detrimental effects were observed on the recovered structure, chemical composition, and electrochemical performance of the regenerated cathode material. The regenerated NCM cathode can achieve a capacity of 163.68 mAh/g at 0.1 C and exhibited a high-capacity retention of 85.58 % after cycling for 200 cycles at 0.5 C. Therefore, the hydrothermal-based regeneration method is effective in revitalizing degraded cathode materials, even in the presence of notable Al impurity content, showing great potential for industrial applications.

Carbon Nanotube-Directed 7 GPa Heterocyclic Aramid Fiber and Its Application in Artificial Muscles.

Poly(p-phenylene-benzimidazole-terephthalamide) (PBIA) fibers with excellent mechanical properties are widely used in fields that require impact-resistant materials such as ballistic protection and aerospace. The introduction of heterocycles in polymer chains increases their flexibility and makes it easier to optimize the fiber structure. However, the inadequate orientation of polymer chains is one of the main reasons for the large difference between the measured and theoretical mechanical properties of PBIA fibers. Herein, carbon nanotubes (CNTs) are selected as an orientation seed. Their structural features allow CNTs to orient during the spinning process, which can induce an orderly arrangement of polymers and improve the orientation of the fiber microstructure. To ensure the complete 1D topology of long CNTs (≈10 µm), PBIA is used as an efficient dispersant to overcome dispersion challenges. The p-CNT/PBIA fibers (10 µm single-walled carbon nanotube 0.025 wt%) exhibit an increase of 22% in tensile strength and 23% in elongation, with a maximum tensile strength of 7.01 ± 0.31 GPa and a reinforcement efficiency of 893.6. The artificial muscle fabricated using CNT/PBIA fibers exhibits a 34.8% contraction and a 25% lifting of a 2 kg dumbbell, providing a promising paradigm for high-performance organic fibers as high-load smart actuators.

Dual-Ion Co-Regulation System Enabling High-Performance Electrochemical Artificial Yarn Muscles with Energy-Free Catch States.

Artificial yarn muscles show great potential in applications requiring low-energy consumption while maintaining high performance. However, conventional designs have been limited by weak ion-yarn muscle interactions and inefficient "rocking-chair" ion migration. To address these limitations, we present an electrochemical artificial yarn muscle design driven by a dual-ion co-regulation system. By utilizing two reaction channels, this system shortens ion migration pathways, leading to faster and more efficient actuation. During the charging/discharging process, [Formula: see text] ions react with carbon nanotube yarn, while Li+ ions react with an Al foil. The intercalation reaction between [Formula: see text] and collapsed carbon nanotubes allows the yarn muscle to achieve an energy-free high-tension catch state. The dual-ion coordinated yarn muscles exhibit superior contractile stroke, maximum contractile rate, and maximum power densities, exceeding those of "rocking-chair" type ion migration yarn muscles. The dual-ion co-regulation system enhances the ion migration rate during actuation, resulting in improved performance. Moreover, the yarn muscles can withstand high levels of isometric stress, displaying a stress of 61 times that of skeletal muscles and 8 times that of "rocking-chair" type yarn muscles at higher frequencies. This technology holds significant potential for various applications, including prosthetics and robotics.

Pretension-Free and Self-Recoverable Coiled Artificial Muscle Fibers with Powerful Cyclic Work Capability.

Similar to natural muscle fibers, coiled artificial muscle fibers provide a straightforward contraction. However, unlike natural muscle fibers, their recovery from the contracted state to the initial state requires high stress, resulting in almost zero work during a full actuation cycle. Herein, a self-recoverable coiled artificial muscle fiber was prepared by conformally coating an elastic carbon nanotube (CNT) fiber with a very thin liquid crystal elastomer (LCE) sheath. The as-obtained muscle fiber demonstrated excellent actuation properties comprising 56.9% contractile stroke, 1522%/s contraction rate, 7.03 kW kg-1 power density, and 32,000 stable cycles. The LCE chains were helically aligned in a nematic phase, and the phase change of the LCE caused by Joule heating drove the actuation process. Moreover, the LCE/CNT fiber had a well-separated, torsionally stable, and elastic coiled structure, which permitted large contractile strokes and acted as an elastic template for external-stress-free recovery. Thus, the use of self-recoverable muscle fibers to mimic the natural muscles for object dragging, multidirectional bending, and quick striking was demonstrated.

Triggering High Capacity and Superior Reversibility of Manganese Oxides Cathode via Magnesium Modulation for Zn//MnO2 Batteries.

Aqueous zinc-ion batteries (ZIBs) have attracted extensive attention in recent years because of its high volumetric energy density, the abundance of zinc resources, and safety. However, ZIBs still suffer from poor reversibility and sluggish kinetics derived from the unstable cathodic structure and the strong electrostatic interactions between bivalent Zn2+ and cathodes. Herein, magnesium doping into layered manganese dioxide (Mg-MnO2 ) via a simple hydrothermal method as cathode materials for ZIBs is proposed. The interconnected nanoflakes of Mg-MnO2 possess a larger specific surface area compared to pristine δ-MnO2 , providing more electroactive sites and boosting the capacity of batteries. The ion diffusion coefficients of Mg-MnO2 can be enhanced due to the improved electrical conductivity by doped cations and oxygen vacancies in MnO2 lattices. The assembled Zn//Mg-MnO2 battery delivers a high specific capacity of 370 mAh g-1 at a current density of 0.6 A g-1 . Furthermore, the reaction mechanism confirms that Zn2+ insertion occurred after a few cycles of activation reactions. Most important, the reversible redox reaction between Zn2+ and MnOOH is found after several charge-discharge processes, promoting capacity and stability. It believes that this systematic research enlightens the design of high-performance of ZIBs and facilitates the practical application of Zn//MnO2 batteries.

Moisture-Adaptive Contractile Biopolymer-Derived Fibers for Wound Healing Promotion.

The advancement in thermosensitive active hydrogels has opened promising opportunities to dynamic full-thickness skin wound healing. However, conventional hydrogels lack breathability to avoid wound infection and cannot adapt to wounds with different shapes due to the isotropic contraction. Herein, a moisture-adaptive fiber that rapidly absorbs wound tissue fluid and produces a large lengthwise contractile force during the drying process is reported. The incorporation of hydroxyl-rich silica nanoparticles in the sodium alginate/gelatin composite fiber greatly improves the hydrophilicity, toughness, and axial contraction performance of the fiber. This fiber exhibits a dynamic contractile behavior as a function of humidity, generating ≈15% maximum contraction strain or ≈24 MPa maximum isometric contractile stress. The textile knitted by the fibers features excellent breathability and generates adaptive contraction in the target direction during the natural desorption of tissue fluid from the wounds. In vivo animal experiments further demonstrate the advantages of the textiles over traditional dressings in accelerating wound healing.

Artificial neuromuscular fibers by multilayered coaxial integration with dynamic adaption.

Integrating sense in a thin artificial muscle fiber for environmental adaption and actuation path tracing, as a snail tentacle does, is highly needed but still challenging because of the interfacing mismatch between the fiber's actuation and sensing components. Here, we report an artificial neuromuscular fiber by wrapping a carbon nanotube (CNT) fiber core in sequence with an elastomer layer, a nanofiber network, and an MXene/CNT thin sheath, achieving the ingenious sense-judge-act intelligent system in an elastic fiber. The CNT/elastomer components provide actuation, and the sheath enables touch/stretch perception and hysteresis-free cyclic actuation tracing due to its strain-dependent resistance. As a whole, the coaxial structure builds a dielectric capacitor that enables sensitive touchless perception. The key to seamless integration is to use a nanofiber interface that allows the sensing layer to adaptively trace but not restrict actuation. This work provides promising solutions for closed-loop control for future intelligent soft robots.

Stepwise Artificial Yarn Muscles with Energy-Free Catch States Driven by Aluminum-Ion Insertion.

Present artificial muscles have been suffering from poor actuation step precision and the need of energy input to maintain actuated states due to weak interactions between guest and host materials or the unstable structural changes. Herein, these challenges are addressed by deploying a mechanism of reversible faradaic insertion and extraction reactions between tetrachloroaluminate ions and collapsed carbon nanotubes. This mechanism allows tetrachloroaluminate ions as a strong but dynamic "locker" to achieve an energy-free high-tension catch state and programmable stepwise actuation in the yarn muscle. When powered off, the muscle nearly 100% maintained any achieved contractile strokes even under loads up to 96,000 times the muscle weight. The actuation mechanism allowed the programmable control of stroke steps down to 1% during reversible actuation. The isometric stress generated by the yarn muscle (14.6 MPa in maximum, 40 times that of skeletal muscles) was also energy freely lockable and step controllable with high precision. Importantly, when fully charged, the muscle stored energy with a high capacity of 102 mAh g-1, allowing the muscle as a battery to power secondary muscles or other devices.

A Hygroscopic Janus Heterojunction for Continuous Moisture-Triggered Electricity Generators.

Moisture-triggered electricity generator (MEG) harvesting energy from the ubiquity of atmospheric moisture is one of the promising potential candidates for renewable power demand. However, MEG device performance is strongly dependent on the moisture concentration, which results in its large fluctuation of the electrical output. Here, a Janus heterojunction MEG device consisting of nanostructured silicon and hygroscopic polyelectrolyte incorporating hydrophilic carbon nanotube mesh is proposed to enable ambient moisture harvesting and continuous stable electrical output delivery. The nanostructured silicon with a large surface/volume ratio provides strong coupling interaction with water molecules for charge generation. A polyelectrolyte of polydiallyl dimethylammonium chloride (PDDA) can facilitate charge selective transporting and enhance the effectiveness of moisture-absorbing in an arid environment simultaneously. The conductive, porous, and hydrophilic carbon nanotube mesh allows water to be ripped through as well as the generated charges being collected timely. As such, any generated charge carriers in the Janus heterojunction can be efficiently swept toward their respective electrodes, because of the device asymmetric contact. A MEG device continuously delivers an open-circuit voltage of 1.0 V, short-circuit current density of 8.2 µA/cm2, and output power density of 2.2 µW/cm2 under an ambient environment (60% relative humidity, 25 °C), which is a record value over the previously reported values. Furthermore, the infrared thermal measurements also reveal that the moisture-triggered electricity generation power is likely ascribed to surrounding thermal energy collected by the MEG device. Our results provide an insightful rationale for the design of device structure and understanding of the working mechanism of MEG, which is of great importance to promote the efficient electricity conversion induced by moisture in the atmosphere.

Temperature-dependent resistance of carbon nanotube fibers.

Carbon nanotube fibers are highly recommended in the field of temperature sensor application owing to their excellent electrical conductivity and thermal conductivity. Here, this work demonstrated the rapid thermal response behaviour of CNT fibers fabricated by floating catalyst CVD method, which was measured by anin situtechnique based on the CNT film electric heater with excellent electrothermal response properties. The temperature dependences of resistance and structure were both explored. Experimental investigation indicates that the reduction in the inter-CNT interspace in the fibers caused by thermally driven actuation was dominantly responsible for the decrease of the fibers resistance during the heating process. Especially, the heated fibers showed 7.2% decrease in electrical resistance at the applied square-wave voltage of 8 V, and good temperature sensitivity (-0.15% °C-1). The as-prepared CNT fibers also featured a rapid and reversible electrical resistance response behaviour when exposed to external heating stimulation. Additionally, with the increment of temperature and twist-degree, the generated contraction actuation increased, which endowed the CNT fibers with more decrease in electrical resistance. These observations further suggested that the temperature-dependent conduction behavior of the CNT fibers with a high reversibility and repeatability was strongly correlated with their structure response to heat stimulation. As a consequence, the temperature-conduction behavior described here may be applied in other CNT-structured fibers and facilitated the improvement in their temperature-sensing applications.

Self-sensing coaxial muscle fibers with bi-lengthwise actuation.

Artificial muscle fibers as a promising biomimetic actuator are needed for such applications as smart soft robots, muscle function restoration, and physical augmentation. Currently developed artificial muscle fibers have shown attractive performance in contractile and torsional actuations. However, the contractile muscle fibers do not have the capability of stimulus-responsive elongation, and real-time identifying their contractile position by themselves is still challenging. We report herein the preparation of a Ti3C2Tx MXene/single walled carbon-nanotubes (SWCNTs)-coated carbon nanotube (CNT)@polydimethylsiloxane (PDMS) coaxial muscle fiber that integrates the important features of self-position sensing and bi-lengthwise actuation. The bi-lengthwise actuation is realized by utilizing the large expansion coefficient difference of PDMS in response to solvent and heat, which results in ∼5% maximum elongation by n-heptane adsorption and ∼19% maximum contraction by electric heating under the optimal conditions. Meanwhile, due to the piezoresistive effect of the MXene/SWCNTs layer, the resistance change of this coating layer is almost linearly dependent on the contraction of the coaxial muscle fiber, providing a function of real-time self-position sensing. Furthermore, an application of using a bundle of these multifunctional coaxial muscle fibers for a bionic arm has been demonstrated, which provides new insights into the design of integrated intelligent artificial muscles with synergistic multiple functions.

Asymmetric Charged Conductive Porous Films for Electricity Generation from Water Droplets via Capillary Infiltrating.

Hydrovoltaic devices are proposed as an alternative way to directly generate electricity due to the ubiquity of water and its interaction with specific porous structures. At present, the output power density of the reported device is limited by its low current density arising from the low surface charge density and inferior charge transport capability of the active materials. In this work, an asymmetric structure consisting of positively charged conductive polyaniline (PANI) and negatively charged Ti3C2TX MXene is proposed to build a hydrovoltaic device to achieve high conductivity and surface charge density simultaneously. An extra polyvinyl alcohol layer is utilized between PANI and MXene to reserve the asymmetric structure and maintain a constant voltage output. As a result, a peak current density of 1.8 mA/cm2 is achieved, which is 18 times higher than the previous peak current density of the device with an inert electrode. Our work of incorporating an asymmetric structure provides an alternative way to target high-efficiency hydrovoltaic devices with a large current density.

Programmable Contractile Actuations of Twisted Spider Dragline Silk Yarns.

The contraction behavior of spider dragline silk upon water exposure has drawn particular interest in developing humidity-responsive smart materials. We report herein that the spider dragline silk yarns with moderate twists can generate much improved lengthwise contraction of 60% or an isometric stress of 11 MPa when wetted by water. Upon the removal of the absorbed water, the dried and contracted spider silk yarns showed programmable contractile actuations. These yarns can be plastically stretched to any specified lengths between the fully contracted state and the state before supercontraction and return to the fully contracted state when wetted. Moreover, the generated isometric stress of these yarns is also programmable, depending on the stretching ratio. The mechanism of the programmable reversible contraction is based on the plastic mechanical property of the dried and contracted spider silk yarns, which can be explained by the variation of the hydrogen bonds and the secondary structures of the proteins in spider dragline silk. Humidity alarm switches, smart doors, and wound healing devices based on the programmable contractile actuations of the spider silk yarns were demonstrated, which provide application scenarios for the supercontraction of spider dragline silk.

Strong and Robust Electrochemical Artificial Muscles by Ionic-Liquid-in-Nanofiber-Sheathed Carbon Nanotube Yarns.

To address the lack of a suitable electrolyte that supports the stable operation of the electrochemical yarn muscles in air, an ionic-liquid-in-nanofibers sheathed carbon nanotube (CNT) yarn muscle is prepared. The nanofibers serve as a separator to avoid the short-circuiting of the yarns and a reservoir for ionic liquid. The ionic-liquid-in-nanofiber-sheathed yarn muscles are strong, providing an isometric stress of 10.8 MPa (about 31 times the skeletal muscles). The yarn muscles are highly robust, which can reversibly contract stably at such conditions as being knotted, wide-range humidity (30 to 90 RH%) and temperature (25 to 70 °C), and long-term cycling and storage in air. By utilizing the accumulated isometric stress, the yarn muscles achieve a high contraction rate of 36.3% s-1 . The yarn muscles are tightly bundled to lift heavy weights and grasp objects. These unique features can make the strong and robust yarn muscles as a desirable actuation component for robotic devices.

Rational and wide-range tuning of CNT aerogel conductors with multifunctionalities.

Different from conventional conductors, elastic 3D nanoarchitectured conductors have shown promise in developing various flexible devices. However, rational design and control of their microstructures to achieve desired physicochemical properties is challenging and lacks comprehensive and profound investigation. In this study, we report an interesting quantitative correlation between density and physical properties when highly porous CNT aerogels are densified, enabling a wide-range tuning of CNT 3D networked structures with different functions. Upon densification by compressing the original thickness of a CNT aerogel by 100 fold, a linear double-logarithmic structure-property relationship in terms of both thickness and density is witnessed, with the resultant density increased by a factor of 100 from 3 to 286 mg cm-3, Young's modulus by 20 times (5.0-105 kPa), electrical conductivity by 400 times (0.4-163 s cm-1), and thermal conductivity by 140 times (0.048-6.7 W m-1 K-1). It can be thus inferred that the CNT aerogel can be regulated with desired mechanical, electrical and thermal properties in a quantitative manner over a wide range, making it promising as a multifunctional aerogel conductor. As a proof, two pieces of CNT aerogel conductors tailored with high conductivity and low thermal conductivity are employed to fabricate a flexible TE device using a simple all-carbon design, which yields a typical power density of 27.5 µW cm-2 and stable outputs under various deformations, demonstrating a potential strategy for design and fabrication of low-cost, flexible and portable power-generation devices.

High-Loading Boron Nitride-Based Bio-Inspired Paper with Plastic-like Ductility and Metal-like Thermal Conductivity.

Although desirable in next-generation flexible electronics, fabricating hybrid film materials with excellent integration of mechanical and thermally conductive yet electrically insulating properties is still a challenge. In mollusk nacre, a small volume of the chitin nanofiber framework hosts 95 vol % CaCO3 microplatelets, enabling the high-loading natural composites to exhibit a ductile deformation behavior. Inspired by this, we fabricate a large-area, boron nitride-based bio-inspired paper using a facile sol-gel-film conversion approach, in which BN microplatelets with a loading of 40-80 wt % are embedded into a 3D poly(p-phenylene benzobisoxazole) nanofiber framework. Because of the vital role of the 3D nanofiber framework, the BN-based paper exhibits plastic-like ductility (38-80%), ultrahigh toughness (10-100 MJ m-3), and good folding endurance. The high-loading BN platelets form an oriented, percolative network and endow the paper with outstanding in-plane thermal conductivity (77.1-214.2 W m-1 K-1) comparable to that of some metals, such as aluminum alloys (108-230 W m-1 K-1). Using the electrically insulating BN-based paper as a flexible substrate, we demonstrate its promising application for lowering the temperature of electronic devices.

Atomic Modulation of 3D Conductive Frameworks Boost Performance of MnO2 for Coaxial Fiber-Shaped Supercapacitors.

Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices. Yet, they are still struggling from inferior energy density, which comes from the limited choices in materials and structure used. Here, Zn-doped CuO nanowires were designed as 3D framework for aligned distributing high mass loading of MnO2 nanosheets. Zn could be introduced into the CuO crystal lattice to tune the covalency character and thus improve charge transport. The Zn-CuO@MnO2 as positive electrode obtained superior performance without sacrificing its areal and gravimetric capacitances with the increasing of mass loading of MnO2 due to 3D Zn-CuO framework enabling efficient electron transport. A novel category of free-standing asymmetric coaxial fiber-shaped supercapacitor based on Zn0.11CuO@MnO2 core electrode possesses superior specific capacitance and enhanced cell potential window. This asymmetric coaxial structure provides superior performance including higher capacity and better stability under deformation because of sufficient contact between the electrodes and electrolyte. Based on these advantages, the as-prepared asymmetric coaxial fiber-shaped supercapacitor exhibits a high specific capacitance of 296.6 mF cm-2 and energy density of 133.47 µWh cm-2. In addition, its capacitance retention reaches 76.57% after bending 10,000 times, which demonstrates as-prepared device's excellent flexibility and long-term cycling stability.