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.     

Ag Nanowire Reinforced Highly Stretchable Conductive Fibers for Wearable Electronics

Stretchable conductive fibers have received significant attention due to their possibility of being utilized in wearable and foldable electronics. Here, highly stretchable conductive fiber composed of silver nanowires (AgNWs) and silver nanoparticles (AgNPs) embedded in a styrene–butadiene–styrene (SBS) elastomeric matrix is fabricated. An AgNW‐embedded SBS fiber is fabricated by a simple wet spinning method. Then, the AgNPs are formed on both the surface and inner region of the AgNW‐embedded fiber via repeated cycles of silver precursor absorption and reduction processes. The AgNW‐embedded conductive fiber exhibits superior initial electrical conductivity (σ₀ = 2450 S cm^?1) and elongation at break (900% strain) due to the high weight percentage of the conductive fillers and the use of a highly stretchable SBS elastomer matrix. During the stretching, the embedded AgNWs act as conducting bridges between AgNPs, resulting in the preservation of electrical conductivity under high strain (the rate of conductivity degradation, σ/σ₀ = 4.4% at 100% strain). The AgNW‐embedded conductive fibers show the strain‐sensing behavior with a broad range of applied tensile strain. The AgNW reinforced highly stretchable conductive fibers can be embedded into a smart glove for detecting sign language by integrating five composite fibers in the glove, which can successfully perceive human motions.     

Highly Stretchable Conducting SIBS‐P3HT Fibers

Poly(styrene‐β‐isobutylene‐β‐styrene)‐poly(3‐hexylthiophene) (SIBS‐P3HT) conducting composite fibers are successfully produced using a continuous flow approach. Composite fibers are stiffer than SIBS fibers and able to withstand strains of up 975% before breaking. These composite fibers exhibit interesting reversible mechanical and electrical characteristics, which are applied to demonstrate their strain gauging capabilities. This will facilitate their potential applications in strain sensing or elastic electrodes. Here, the fabrication and characterization of highly stretchable electrically conducting SIBS‐P3HT fibers using a solvent/non‐solvent wet‐spinning technique is reported. This fabrication method combines the processability of conducting SIBS‐P3HT blends with wet‐spinning, resulting in fibers that could be easily spun up to several meters long. The resulting composite fiber materials exhibit an increased stiffness (higher Young’s modulus) but lower ductility compared to SIBS fibers. The fibers’ reversible mechanical and electrical characteristics are applied to demonstrate their strain gauging capabilities.     

Reversible Crumpling of 2D Titanium Carbide (MXene) Nanocoatings for Stretchable Electromagnetic Shielding and Wearable Wireless Communication

In the emerging Internet of Things, stretchable antennas can facilitate wireless communication between wearable and mobile electronic devices around the body. The proliferation of wireless devices transmitting near the human body also raises interference and safety concerns that demand stretchable materials capable of shielding electromagnetic interference (EMI). Here, an ultrastretchable conductor is fabricated by depositing a crumple‐textured coating composed of 2D Ti₃C₂T_x nanosheets (MXene) and single‐walled carbon nanotubes (SWNTs) onto latex, which can be fashioned into high‐performance wearable antennas and EMI shields. The resulting MXene‐SWNT (S‐MXene)/latex devices are able to sustain up to an 800% areal strain and exhibit strain‐insensitive resistance profiles during a 500‐cycle fatigue test. A single layer of stretchable S‐MXene conductors demonstrate a strain‐invariant EMI shielding performance of ≈30 dB up to 800% areal strain, and the shielding performance is further improved to ≈47 and ≈52 dB by stacking 5 and 10 layers of S‐MXene conductors, respectively. Additionally, a stretchable S‐MXene dipole antenna is fabricated, which can be uniaxially stretched to 150% with unaffected reflected power <0.1%. By integrating S‐MXene EMI shields with stretchable S‐MXene antennas, a wearable wireless system is finally demonstrated that provides mechanically stable wireless transmission while attenuating EM absorption by the human body.     

Coaxial Thermoplastic Elastomer‐Wrapped Carbon Nanotube Fibers for Deformable and Wearable Strain Sensors

Highly conductive and stretchable fibers are crucial components of wearable electronics systems. Excellent electrical conductivity, stretchability, and wearability are required from such fibers. Existing technologies still display limited performances in these design requirements. Here, achieving highly stretchable and sensitive strain sensors by using a coaxial structure, prepared via coaxial wet spinning of thermoplastic elastomer‐wrapped carbon nanotube fibers, is proposed. The sensors attain high sensitivity (with a gauge factor of 425 at 100% strain), high stretchability, and high linearity. They are also reproducible and durable. Their use as safe sensing components on deformable cable, expandable surfaces, and wearable textiles is demonstrated.     

Knittable and Washable Multifunctional MXene‐Coated Cellulose Yarns

Textile‐based electronics enable the next generation of wearable devices, which have the potential to transform the architecture of consumer electronics. Highly conductive yarns that can be manufactured using industrial‐scale processing and be washed like everyday yarns are needed to fulfill the promise and rapid growth of the smart textile industry. By coating cellulose yarns with Ti₃C₂T_x MXene, highly conductive and electroactive yarns are produced, which can be knitted into textiles using an industrial knitting machine. It is shown that yarns with MXene loading of ≈77 wt% (≈2.2 mg cm^?1) have conductivity of up to 440 S cm^?1. After washing for 45 cycles at temperatures ranging from 30 to 80 °C, MXene‐coated cotton yarns exhibit a minimal increase in resistance while maintaining constant MXene loading. The MXene‐coated cotton yarn electrode offers a specific capacitance of 759.5 mF cm^?1 at 2 mV s^?1. A fully knitted textile‐based capacitive pressure sensor is also prepared, which offers high sensitivity (gauge factor of ≈6.02), wide sensing range of up to ≈20% compression, and excellent cycling stability (2000 cycles at ≈14% compression strain). This work provides new and practical insights toward the development of platform technology that can integrate MXene in cellulose‐based yarns for textile‐based devices.     

A Self‐Healable,Highly Stretchable,and Solution Processable Conductive Polymer Composite for Ultrasensitive Strain and Pressure Sensing

Mimicking human skin's functions to develop electronic skins has inspired tremendous efforts in design and synthesis of novel soft materials with simplified fabrication methods. However, it still remains a great challenge to develop electronically conductive materials that are both stretchable and self‐healable. Here it is demonstrated that a ternary polymer composite comprised of polyaniline, polyacrylic acid, and phytic acid can exhibit high stretchability ( ≈ 500%) and excellent self‐healing properties. The polymer composite with optimized composition shows an electrical conductivity of 0.12 S cm^?1. On rupture, both electrical and mechanical properties can be restored with ≈ 99% efficiency in a 24 h period, which is enabled by the dynamic hydrogen bonding and electrostatic interactions. It is further shown that this composite is both strain and pressure sensitive, and therefore can be used for fabricating strain and pressure sensors to detect a variety of mechanical deformations with ultrahigh sensitivity. The sensitivity and sensing range are the highest among all of the reported self‐healable piezoresistive pressure sensors and even surpass most flexible mechanical sensors. Notably, this composite is prepared via a solution casting process, which potentially allows for large‐area, low‐cost fabrication electronic skins.     

Ionoskins: Nonvolatile,Highly Transparent,Ultrastretchable Ionic Sensory Platforms for Wearable Electronics

The primary technology of next‐generation wearable electronics pursues the development of highly deformable and stable systems. Here, nonvolatile, highly transparent, and ultrastretchable ionic conductors based on polymeric gelators [poly(methyl methacrylate‐ran‐butyl acrylate), PMMA‐r‐PBA] and ionic liquids (IL) are proposed. A crucial strategy in the molecular design of polymer gelators is copolymerization of PMMA and IL‐insoluble low glass transition temperature (T_g) polymers that can be deformed and effectively dissipate applied strains. Highly stretchable (elongation limit ≈850%), mechanically robust (elastic modulus ≈3.1 × 10⁵ Pa), and deformation durable (recovery ratio ≈96.1% after 500 stretching/releasing cycles) gels are obtained by judiciously adjusting the molecular characteristics of polymer gelators and gel composition. An extremely simple “ionic” strain sensory platform is fabricated by directly connecting the stretchable gel and a digital multimeter, exhibiting high sensitivity (gauge factor ≈2.73), stable operation (>13 000 cycles), and nonvolatility (>10 d in air). Moreover, the skin‐type strain sensor, referred to as ionoskin, is demonstrated. The gels are attached to a part of the body (e.g., finger, elbow, knee, or ankle) and various human movements are successfully monitored. The ionoskin renders the opportunity to achieve wearable ubiquitous electronics such as healthcare devices and smart textile systems.     

Highly Flexible and Stretchable Nanowire Superlattice Fibers Achieved by Spring‐Like Structure of Sub‐1 nm Nanowires

Conventional inorganic nanowire (NW) fibers are usually not stretchable and elastic, which may limit their practical applications. Inspired by the similarity between inorganic sub‐1 nm NWs and polymer chains in dimension, and helical spring‐like structure of cellulose in cherry bark, highly flexible and stretchable NW superlattice fibers composed of sub‐1 nm GdOOH NWs are fabricated. The NW fibers could be twined, bent, twisted, and tied without any damage. When the strain is less than 10%, the fibers present elastic deformation. The elongation at break of the fibers usually reaches ≈40–50% and the highest elongation could reach ≈86%. Excellent flexibility and stretchability of the NW fibers are attributed to the well‐aligned spring‐like NWs assembled superlattice, which are demonstrated by scanning electron microscopy tests, synchrotron small‐angle X‐ray scattering, and obvious birefringence. Moreover, NW‐nanoparticle (NP) fibers are fabricated, inspired by inorganic nanoparticle–reinforced polymers. The strength is improved compared with the NW fibers. Based on this work, it is possible to fabricate multifunctional, flexible, and stretchable inorganic NW materials composed of different inorganic sub‐1 nm NWs, which may be useful in practical applications.     

Stretchable Conductive Composites Based on Metal Wools for Use as Electrical Vias in Soft Devices

Soft devices can be bent, stretched, and compressed reversibly, but conventional wires are rigid. This work describes stretchable composites that are easily fabricated with simple tools and commodity materials, and that can provide a strategy for electrical wiring that meets certain needs of soft devices. These composites are made by combining metal wool and elastomeric polymers. Embedding fine (average fiber width ≈25 μm) steel wool (or other metal wools) in a silicone polymer creates an electrically conductive path through the nonconductive elastomer. This composite is flexible, stretchable, compressible, inexpensive, and simple to incorporate into the bodies of soft devices. It is also electrically anisotropic, and shows maximum conductivity along the majority axis of the fibers, but maximum extension perpendicular to this axis. The utility of this composite for creating an electrically conductive path through an elastomer was demonstrated in several devices, including: a soft, solderless breadboard, a soft touch sensor, and a soft strain gauge.     

Stretchable,Skin‐Mountable,and Wearable Strain Sensors and Their Potential Applications: A Review

There is a growing demand for flexible and soft electronic devices. In particular, stretchable, skin‐mountable, and wearable strain sensors are needed for several potential applications including personalized health‐monitoring, human motion detection, human‐machine interfaces, soft robotics, and so forth. This Feature Article presents recent advancements in the development of flexible and stretchable strain sensors. The article shows that highly stretchable strain sensors are successfully being developed by new mechanisms such as disconnection between overlapped nanomaterials, crack propagation in thin films, and tunneling effect, different from traditional strain sensing mechanisms. Strain sensing performances of recently reported strain sensors are comprehensively studied and discussed, showing that appropriate choice of composite structures as well as suitable interaction between functional nanomaterials and polymers are essential for the high performance strain sensing. Next, simulation results of piezoresistivity of stretchable strain sensors by computational models are reported. Finally, potential applications of flexible strain sensors are described. This survey reveals that flexible, skin‐mountable, and wearable strain sensors have potential in diverse applications while several grand challenges have to be still overcome.     

Smart and Multifunctional Fiber-Reinforced Composites of 2D Heterostructure-Based Textiles

Smart and multifunctional fiber reinforced polymer (FRP) composites with energy storage, sensing, and heating capabilities have gained significant interest for automotive, civil, and aerospace applications. However, achieving smart and multifunctional capabilities in an FRP composite while maintaining desired mechanical properties remains challenging. Here, a novel approach for layer-by-layer (LBL) deposition of 2D material (graphene and molybdenum disulfide, MoS₂)-based heterostructure onto glass fiber fabric using a highly scalable manufacturing technique at a remarkable speed of ≈150 m min⁻¹ is reported. This process enables the creation of smart textiles with integrated energy storage, sensing, and heating functionalities. This methodology combines gel-based electrolyte with a vacuum resin infusion technique, resulting in an efficient and stable smart FRP composite with an areal capacitance of up to ≈182 µF cm⁻² at 10 mV s⁻¹. The composite exhibits exceptional cyclic stability, maintaining ≈90% capacitance after 1000 cycles. Moreover, the smart composite demonstrates joule heating, reaching from ≈24 to ≈27 °C within 120 s at 25 V. Additionally, the smart composite displays strain sensitivity by altering electrical resistance with longitudinal strain, enabling structural health monitoring. These findings highlight the potential of smart composites for multifunctional applications and provide an important step toward realizing their actual real-world applications.     

Ultrastretchable Fibers with Metallic Conductivity Using a Liquid Metal Alloy Core

The fabrication and characterization of fibers that are ultrastretchable and have metallic electrical conductivity are described. The fibers consist of a liquid metal alloy, eutectic gallium indium (EGaIn), injected into the core of stretchable hollow fibers composed of a triblock copolymer, poly[styrene‐b‐(ethylene‐co‐butylene)‐b‐styrene] (SEBS) resin. The hollow fibers are easy to mass‐produce with controlled size using commercially available melt processing methods. The fibers are similar to conventional metallic wires, but can be stretched orders of magnitude further while retaining electrical conductivity. Mechanical measurements with and without the liquid metal inside the fibers show the liquid core has a negligible impact on the mechanical properties of the fibers, which is in contrast to most conductive composite fibers. The fibers also maintain the same tactile properties with and without the metal. Electrical measurements show that the fibers increase resistance as the fiber elongates and the cross sectional area narrows. Fibers with larger diameters change from a triangular to a more circular cross‐section during stretching, which has the appeal of lowering the resistance below that predicted by theory. To demonstrate their utility, the ultrastretchable fibers are used as stretchable wires for earphones and for a battery charger and perform as well as their conventional parts.     

A Wrinkled PEDOT:PSS Film Based Stretchable and Transparent Triboelectric Nanogenerator for Wearable Energy Harvesters and Active Motion Sensors

The functionalized conductive polymer is a promising choice for flexible triboelectric nanogenerators (TENGs) for harvesting human motion energy still poses challenges. In this work, a transparent and stretchable wrinkled poly(3,4‐ethylenedioxythiophene):poly(4‐styrenesulfonate) (PEDOT:PSS) electrode based TENG (WP‐TENG) is fabricated. The optimum conductivity and transparency of PEDOT:PSS electrode can reach 0.14 kΩ □⁻¹ and 90%, respectively, with maximum strain of ≈100%. Operating in single‐electrode mode at 2.5 Hz, the WP‐TENG with an area of 6 × 3 cm² produces an open‐circuit voltage of 180 V, short‐circuit current of 22.6 µA, and average power density of 4.06 mW m⁻². It can be worn on the wrist to harvest hand tapping energy and charge the capacitor to 2 V in ≈3.5 min, and then drive an electronic watch. Furthermore, the WP‐TENG as the human motion monitoring sensor could inspect the bending angle of the elbow and joint by analyzing the peak value of voltage and monitor the motion frequency by counting the peak number. The triboelectric mechanism also enables the WP‐TENG to realize high‐performance active tactile sensing. The assembled 3 pixel × 3 pixel tactile sensor array is fabricated for mapping the touch location or recording the shape of object contacted with the sensor array.     

Stretchable and Self-Healable Semiconductive Composites Based on Hydrogen Bonding Cross-linked Elastomeric Matrix

Semiconductors with both high stretchability and self-healing capability are highly desirable for various wearable devices. Much progress has been achieved in designing highly stretchable semiconductive polymers or composites. The demonstration of self-healable semiconductive composite is still rare. Here, an extremely soft, highly stretchable, and self-healable hydrogen bonding cross-linked elastomer, amide functionalized-polyisobutylene (PIB-amide) is developed, to enable a self-healable semiconductive composite through compounding with a high-performance conjugated diketopyrrolopyrrole (DPP-T) polymer. The composite, consisting of 20% DPP-T and 80% PIB-amide, shows record high crack-onset strain (COS ≈1500%), extremely low elastic modulus (E≈1.6 MPa), and unique ability to spontaneously self-heal atroom temperature within 5 min. Unlike previous works, these unique composite materials also show strain-independent charge mobility. An in-depth morphological study based on multi-model techniques indicate that all composites show blending ratio- and stretching-independent fibril-like aggregation due to the strong hydrogen bond in elastomer to enable the unique stable charge mobility. This study provides a new direction to develop highly healable and electronically stable semiconductive composite and will enable new applications of stretchable electronics.     

Block Copolymer-Based Supramolecular Ionogels for Accurate On-Skin Motion Monitoring

Interest in wearable and stretchable on-skin motion sensors has grown rapidly in recent years. To expand their applicability, the sensing element must accurately detect external stimuli; however, weak adhesiveness of the sensor to a target object has been a major challenge in developing such practical and versatile devices. In this study, freestanding, stretchable, and self-adhesive ionogel conductors are demonstrated which are composed of an associating polymer network and ionic liquid that enable conformal contact between the sensor and skin even during dynamic movement. The network of ionogel is formed by noncovalent association of two diblock copolymers, where phase-separated micellar clusters are interconnected via hydrogen bonds between corona blocks. The resulting ionogels exhibit superior adhesive characteristics, including a very high lift-off force of 93.3 N m⁻¹, as well as excellent elasticity (strain at break ≈ 720%), toughness ( ≈ 2479 kJ m⁻³), thermal stability ( ≈ 150  ° C), and high ionic conductivity ( ≈ 17.8 mS cm⁻¹ at 150  ° C). These adhesive ionogels are successfully applied to stretchable on-skin strain sensors as sensing elements. The resulting devices accurately monitor the movement of body parts such as the wrist, finger, ankle, and neck while maintaining intimate contact with the skin, which was not previously possible with conventional non-adhesive ionogels.     

A Skin‐Inspired Substrate with Spaghetti‐Like Multi‐Nanofiber Network of Stiff and Elastic Components for Stretchable Electronics

Mimicking the skin's non‐linear self‐limiting mechanical characteristics is of great interest. Skin is soft at low strain but becomes stiff at high strain and thereby can protect human tissues and organs from high mechanical loads. Herein, the design of a skin‐inspired substrate is reported based on a spaghetti‐like multi‐nanofiber network (SMNN) of elastic polyurethane (PU) nanofibers (NFs) sandwiched between stiff poly(vinyldenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) NFs layers embedded in polydimethylsiloxane elastomer. The elastic moduli of the stretchable skin‐inspired substrate can be tuned in a range that matches well with the mechanical properties of skins by adjusting the loading ratios of the two NFs. Confocal imaging under stretching indicates that PU NFs help maintain the stretchability while adding stiff P(VDF‐TrFE) NFs to control the self‐limiting characteristics. Interestingly, the Au layer on the substrate indicates a negligible change in the resistance under cyclic (up to 7000 cycles at 35% strain) and dynamic stretching (up to 35% strain), which indicates the effective absorption of stress by the SMNN. A stretchable chemoresistive gas sensor on the skin‐inspired substrate also demonstrates a reasonable stability in NO₂ sensing response under strain up to 30%. The skin‐inspired substrate with SMNN provides a step toward ultrathin stretchable electronics.     

Stretchable and Temperature‐Sensitive Polymer Optical Fibers for Wearable Health Monitoring

Stretchable physical sensors that can detect and quantify human physiological signals such as temperature, are essential to the realization of healthcare devices for biomedical monitoring and human–machine interfaces. Despite recent achievements in stretchable electronic sensors using various conductive materials and structures, the design of stretchable sensors in optics remains a considerable challenge. Here, an optical strategy for the design of stretchable temperature sensors, which can maintain stable performance even under a strain deformation up to 80%, is reported. The optical temperature sensor is fabricated by the incorporation of thermal‐sensitive upconversion nanoparticles (UCNPs) in stretchable polymer‐based optical fibers (SPOFs). The SPOFs are made from stretchable elastomers and constructed in a step‐index core/cladding structure for effective light confinements. The UCNPs, incorporated in the SPOFs, provide thermal‐sensitive upconversion emissions at dual wavelengths for ratiometric temperature sensing by near‐infrared excitation, while the SPOFs endow the sensor with skin‐like mechanical compliance and excellent light‐guiding characteristics for laser delivery and emission collection. The broad applications of the proposed sensor in real‐time monitoring of the temperature and thermal activities of the human body, providing optical alternatives for wearable health monitoring, are demonstrated.     

All‐Solid‐State Asymmetric Supercapacitors with Metal Selenides Electrodes and Ionic Conductive Composites Electrolytes

All‐solid‐state flexible asymmetric supercapacitors (ASCs) are developed by utilization of graphene nanoribbon (GNR)/Co_0.85Se composites as the positive electrode, GNR/Bi₂Se₃ composites as the negative electrode, and polymer‐grafted‐graphene oxide membranes as solid‐state electrolytes. Both GNR/Co_0.85Se and GNR/Bi₂Se₃ composite electrodes are developed by a facile one‐step hydrothermal growth method from graphene oxide nanoribbons as the nucleation framework. The GNR/Co_0.85Se composite electrode exhibits a specific capacity of 76.4 mAh g^?1 at a current density of 1 A g^?1 and the GNR/Bi₂Se₃ composite electrode exhibits a specific capacity of 100.2 mAh g^?1 at a current density of 0.5 A g^?1. Moreover, the stretchable membrane solid‐state electrolytes exhibit superior ionic conductivity of 108.7 mS cm^?1. As a result, the flexible ASCs demonstrate an operating voltage of 1.6 V, an energy density of 30.9 Wh kg^?1 at the power density of 559 W kg^?1, and excellent cycling stability with 89% capacitance retention after 5000 cycles. All these results demonstrate that this study provides a simple, scalable, and efficient approach to fabricate high performance flexible all‐solid‐state ASCs for energy storage.     

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.