Piezoelectric Nylon-11 Fibers for Electronic Textiles,Energy Harvesting and Sensing

Electronic textiles and functional fabrics are among the key constituents envisioned for wearable electronics applications. For e-textiles, the challenge is to process materials of desired electronic properties such as piezoelectricity into fibers to be integrated as wefts or wraps in the fabrics. Nylons, first introduced in the 1940s for stockings, are among the most widely used synthetic fibers in textiles. However, realization of nylon-based e-textiles has remained elusive due to the difficulty of achieving the piezoelectric phase in the nylon fibers. Here, piezoelectric nylon-11 fibers are demonstrated and it is shown that the resulting fibers are viable for applications in energy harvesting from low frequency mechanical vibrations and in motion sensors. A simulation study is presented that elucidates on the sensitivity of the nylon-11 fibers toward external mechanical stimuli. Moreover, a strategy is proposed and validated to significantly boost the electrical performance of the fibers. Since a large fraction of the textile industry is based on nylon fibers, the demonstration of piezoelectric nylon fibers will be a major step toward realization of electronic textiles for applications in apparels, health monitoring, sportswear, and portable energy generation.     

Advances in Wearable Strain Sensors Based on Electrospun Fibers

Wearable strain sensors with the ability of detecting physiological activities play an important role in personalized healthcare. Electrospun fibers have become a popular building block for wearable strain sensors due to their excellent mechanical properties, breathability, and light weight. In this review, the structure and preparation process of electrospun fibers and the conductive layer are systematically introduced. The impact of materials and structures of electrospun fibers on the wearable strain sensors with a following discussion of sensing performance optimization strategies is outlined. Furthermore, the applications of electrospun fiber-based wearable strain sensors in biomonitoring, motion detection, and human-machine interaction are presented. Finally, the challenges and promising future directions for the community of wearable strain sensors based on electrospun fibers are pointed out.     

Theoretical Model and Outstanding Performance from Constructive Piezoelectric and Triboelectric Mechanism in Electrospun PVDF Fiber Film

Flexible materials with high electromechanical coupling performance are highly demanded for wide applications for electromechanical sensors and transducers, including mechanical energy harvesters. Here, outstanding electromechanical performance is obtained in electrospun‐aligned polyvinylidene fluoride (PVDF) fiber film. A theoretical model is developed from systematic theoretical analyses to clarify the underlying constructive piezoelectric‐triboelectric mechanism in the polarized PVDF fiber films that explains the experimental observations well. The electrospinning process induces polarization alignment and thus tunes the electron affinity for PVDF fibers with different polarization terminals, which results in the constructive piezoelectric and triboelectric responses in the obtained PVDF fiber films. Extremely large effective piezoelectric performance properties are achieved in the direct piezoelectric measurements, reaching the maximum effective piezoelectric strain and voltage coefficients of ?1065 pm V^?1 and ?9178 V mm N^?1, respectively, at 100 Hz. In the converse piezoelectric measurements without a significant contribution from reversible triboelectric effect, the maximum effective piezoelectric strain and voltage coefficients are ?166 pm V^?1 and ?1499 V mm N^?1, respectively. The theoretical analyses and experimental results show the great potential of the electrospun aligned polar PVDF fiber material for various electromechanical device applications, particularly for mechanical energy harvesting.     

Conductive MXene Nanocomposite Organohydrogel for Flexible,Healable, Low‐Temperature Tolerant Strain Sensors

Conductive hydrogels are attracting tremendous interest in the field of flexible and wearable soft strain sensors because of their great potential in electronic skins, and personalized healthcare monitoring. However, conventional conductive hydrogels using pure water as the dispersion medium will inevitably freeze at subzero temperatures, resulting in the diminishment of their conductivity and mechanical properties; meanwhile, even at room temperature, such hydrogels suffer from the inevitable loss of water due to evaporation, which leads to a poor shelf‐life. Herein, an antifreezing, self‐healing, and conductive MXene nanocomposite organohydrogel (MNOH) is developed by immersing MXene nanocomposite hydrogel (MNH) in ethylene glycol (EG) solution to replace a portion of the water molecules. The MNH is prepared from the incorporation of the conductive MXene nanosheet networks into hydrogel polymer networks. The as‐prepared MNOH exhibits an outstanding antifreezing property (?40 °C), long‐lasting moisture retention (8 d), excellent self‐healing capability, and superior mechanical properties. Furthermore, this MNOH can be assembled as a wearable strain sensor to detect human biologic activities with a relatively broad strain range (up to 350% strain) and a high gauge factor of 44.85 under extremely low temperatures. This work paves the way for potential applications in electronic skins, human?machine interactions, and personalized healthcare monitoring.     

Multifunctional Fiber for Synchronous Bio-Sensing and Power Supply in Sweat Environment

Continuous monitoring of human sweat, which enables highly sensitive multiple biomarkers analysis with a portable power supply, is increasingly desired for the remote healthcare industry. Smart fibers with on-demand functionality are ideal candidates for fabricating noninvasive and conformal bioelectronic devices owing to their considerable flexibility. Herein, a multifunctional textile patch based on a reduced graphene oxide (rGO)/tetra-aniline (TANi) fiber for simultaneous biomarker monitoring and energy supply is reported. Benefiting from the multi-electrochemical redox states and proton doping/dedoping characteristics of TANi, rGO/TANi hybrid fibers are combined into an energy storage device and biosensor in a physiological environment. GO flakes increase the viscoelasticity of the wet-spinning dope by regulating the noncovalent interactions between TANi aggregates, thereby enhancing the mechanical strength and conductivity of the resulting rGO/TANi hybrid fiber. Consequently, the hybrid fiber exhibits high volumetric capacitance and versatile sensing capability for various physiological analytes, e.g., pH, K⁺, and glucose in sweat electrolyte. Furthermore, a wireless continuous sweat monitoring system is constructed by integrating the multifunctional fiber sensor into a printed electric circuit board with programmed functionality. Such a delicate integrated design that harnesses the signal collection and communication units is anticipated to facilitate practical applications in personalized diagnostic and physiological health.     

Nonwoven fabric active electrodes for biopotential measurement during normal daily activity

Body movement is responsible for most of the interference during physiological data acquisition during normal daily activities. In this paper, we introduce nonwoven fabric active electrodes that provide the comfort required for clothing while robustly recording physiological data in the presence of body movement. The nonwoven fabric active electrodes were designed and fabricated using both hand- and screen-printing thick-film techniques. Nonstretchable nonwoven (Evolon 100) was chosen as the flexible fabric substrate and a silver filled polymer ink (Creative Materials CMI 112-15) was used to form a transducer layer and conductive lines on the nonwoven fabrics. These nonwoven fabric active electrodes can be easily integrated into clothing for wearable health monitoring applications. Test results indicate that nonwoven textile-based sensors show considerable promise for physiological data acquisition in wearable healthcare monitoring applications.     

Recent Progress on Structure Manipulation of Poly(vinylidene fluoride)-Based Ferroelectric Polymers for Enhanced Piezoelectricity and Applications

Poly(vinylidene fluoride) (PVDF)-based polymers demonstrate great potential for applications in flexible and wearable electronics but show low piezoelectric coefficients (e.g., −d₃₃ < 30 pC N⁻¹). The effective improvement for the piezoelectricity of PVDF is achieved by manipulating its semicrystalline structures. However, there is still a debate about which component is the primary contributor to piezoelectricity. Therefore, current methods to improve the piezoelectricity of PVDF can be classified into modulations of the amorphous phase, the crystalline region, and the crystalline–amorphous interface. Here, the basic principles and measurements of piezoelectric coefficients for soft polymers are first discussed. Then, three different categories of structural modulations are reviewed. In each category, the physical understanding and strategies to improve the piezoelectric performance of PVDF are discussed. In particular, the crucial role of the oriented amorphous fraction at the crystalline–amorphous interface in determining the piezoelectricity of PVDF is emphasized. At last, the future development of high performance piezoelectric polymers is outlooked.     

Environment friendly,transparent nanofiber textiles consolidated with high efficiency PLEDs for wearable electronics

Electrospinning used to fabricate eco-friendly, transparent, human hair-based nanofibers (NFs) using natural resources such as keratin (which is found in hair, wool, feather, nails, and horns). These NF-based textiles are very useful in making transparent, wearable electronics, as they possess unique optical properties in the visible light regions, such as transparency exceeding 85%. The resulting environmentally friendly, hair-based NFs were investigated through various methods. In order to study transparent property of optically transparent NFs for applying transparent wearable devices, we fabricated transparent flexible consolidated sandwich structures embedded in NF textiles with polymer light-emitting diodes (PLEDs). The devices exhibit the fabrication process and characterization of consolidated textiles and PLEDs by using various color emission type of polymer. Also, we investigated a comparison between PLEDs without textiles and consolidated PLEDs with textile. When used white, red, and yellow polymer in this consolidated textile/LEDs/textile structures, the performances of device was obtained from a spectrally white, red, and yellow color light with a maximum luminance of 2781, 2430, and 6305 cd/m² at 13, 11, and 10 V, respectively. The LED characteristics of the consolidated PLEDs with textile maintained similar device efficiencies of PLEDs without textiles.     

Piezoelectric Nanogenerator Based on In Situ Growth All-Inorganic CsPbBr3 Perovskite Nanocrystals in PVDF Fibers with Long-Term Stability

Inorganic lead halide perovskite has become an emerging material for modern photoelectric and electronic nanodevices due to its excellent optical and electronic properties. In view of its huge dielectric and electrical properties, inorganic CsPbBr₃ perovskite is introduced into the piezoelectric nanogenerator (PENG). Based on one-step electrospinning of solutions containing CsPbBr₃ precursors and polyvinylidene difluoride (PVDF), in situ growth of CsPbBr₃ nanocrystals in PVDF fibers (CsPbBr₃@PVDF composite fibers) with highly uniform size and spatial distribution are synthesized. The CsPbBr₃@PVDF composite fibers based PENG reveals an open-circuit voltage (V_oc) of 103 V and a density of short-circuit current (I_sc) of 170  µ A cm⁻², where the V_oc is comparable to the state-of-the-art hybrid composite piezoelectric nanogenerators (PENGs) and the density of I_sc is 4.86 times higher than that of lead halide perovskites counterpart ever reported. Moreover, CsPbBr₃@PVDF composite fibers based PENG exhibits fundamentally improved thermal/water/acid–base stabilities. This study suggests that the CsPbBr₃@PVDF composite fiber is a good candidate for fabricating high-performance PENGs, promising application potentials in mechanical energy harvesting and motion sensing technologies.     

Hierarchically Interconnected Piezoceramic Textile with a Balanced Performance in Piezoelectricity,Flexibility, Toughness,and Air Permeability

Softening of piezoelectric materials facilitates the development of flexible wearables and energy harvesting devices. However, as one of the most competitive candidates, piezoelectric ceramic-polymer composites inevitably exhibit reduced power-generation capability and weak mechanical strength due to the mismatch of strength and permittivity between the two phases inside. Herein a flexible, air-permeable, and high-performance piezoceramic textile composite with a mechanically reinforced hierarchical porous structure is introduced. Based on a template-assisted sol-gel method, a three-order hierarchical ceramic textile is constructed by intertwining submillimeter-scale multi-ply ceramic fibers that are further formed by twisting micrometer-scale one-ply ceramic fibrils. Theoretical analysis indicates that large mechanical stress can be easily induced in the multi-order hierarchical structure, which greatly benefits the electrical output. Fabricated samples generate an open-circuit voltage of 128 V, a short-circuit current of 120 µA, and an instantaneous power density of 0.75 mW cm⁻², much higher than the previously reported works. The developed multi-order and 3D-interconnected piezoceramic textile shows satisfactory piezoelectricity (d₃₃ of 190 pm V⁻¹), air permeability (45.1 mm s⁻¹), flexibility (Young's modulus of 0.35 GPa), and toughness (0.125 MJ m⁻³), collectively. The design strategy of obtaining balanced properties promotes the practicality of smart/functional materials in wearables and flexible electronics.     

Multifunctional Smart Textronics with Blow‐Spun Nonwoven Fabrics

Here, the fabrication of nonwoven fabric by blow spinning and its application to smart textronics are demonstrated. The blow‐spinning system is composed of two parallel concentric fluid streams: i) a polymer dissolved in a volatile solvent and ii) compressed air flowing around the polymer solution. During the jetting process with pressurized air, the solvent evaporates, which results in the deposition of nanofibers in the direction of gas flow. Poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVdF‐HFP) dissolved in acetone is blow‐spun onto target substrate. Conductive nonwoven fabric is also fabricated from a blend of single‐walled carbon nanotubes (SWCNTs) and PVdF‐HFP. An all‐fabric capacitive strain sensor is fabricated by vertically stacking the PVdF‐HFP dielectric fabric and the SWCNT/PVdF‐HFP conductive fabric. The resulting sensor shows a high gauge factor of over 130 and excellent mechanical durability. The hierarchical morphology of nanofibers enables the development of superhydrophobic fabric and their electrical and thermal conductivities facilitate the application to a wearable heater and a flexible heat‐dissipation sheet, respectively. Finally, the conductive nonwoven fabric is successfully applied to the detection of various biosignals. The demonstrated facile and cost‐effective fabrication of nonwoven fabric by the blow‐spinning technique provides numerous possibilities for further development of technologies ranging from wearable electronics to textronics.     

A Robust Wearable Point-of-Care CNT-Based Strain Sensor for Wirelessly Monitoring Throat-Related Illnesses

Point-of-care testing (POC) has the ability to detect chronic and infectious diseases early or at the time of occurrence and provide a state-of-the-art personalized healthcare system. Recently, wearable and flexible sensors have been employed to analyze sweat, glucose, blood, and human skin conditions. However, a flexible sensing system that allows for the real-time monitoring of throat-related illnesses, such as salivary parotid gland swelling caused by flu and mumps, is necessary. Here, for the first time, a wearable, highly flexible, and stretchable piezoresistive sensing patch based on carbon nanotubes (CNTs) is reported, which can record muscle expansion or relaxation in real-time, and thus act as a next-generation POC sensor. The patch offers an excellent gauge factor for in-plane stretching and spatial expansion with low hysteresis. The actual extent of muscle expansion is calculated and the gauge factor for applications entailing volumetric deformations is redefined. Additionally, a bluetooth-low-energy system that tracks muscle activity in real-time and transmits the output signals wirelessly to a smartphone app is utilized. Numerical calculations verify that the low stress and strain lead to excellent mechanical reliability and repeatability. Finally, a dummy muscle is inflated using a pneumatic-based actuator to demonstrate the application of the affixed wearable next-generation POC sensor.     

High‐Performance Polypyrrole/Graphene/SnCl2 Modified Polyester Textile Electrodes and Yarn Electrodes for Wearable Energy Storage

Flexible supercapacitors have potential for wearable energy storage due to their high energy/power densities and long operating lifetimes. High electrochemical performance with robust mechanical properties is highly desired for flexible supercapacitor electrodes. Usually, the mechanical properties are improved by choosing high flexible textile substrates but at the much expense of electrochemical performance due to the nonideal contact between conductive materials and textile substrates. Herein, the authors present an efficient, scalable, and general strategy for the simultaneous fabrication of high‐performance textile electrodes and yarn electrodes. It is interesting to find that the conformal reduced graphene oxide (RGO) layer is uniformly and successively painted on the surface of SnCl₂ modified polyester fibers (M‐PEF) via a repeated “dyeing and drying” strategy. The large‐area textile electrodes and ultralong yarn electrodes are fabricated by using RGO/M‐PEF as substrate with subsequent deposition of polypyrrole. This work provides new opportunities for developing high flexible textile electrodes and yarn electrodes with further increased electrochemical performance and scalable production.     

MXene Functionalized,Highly Breathable and Sensitive Pressure Sensors with Multi-Layered Porous Structure

Breathable, flexible, and highly sensitive pressure sensors have drawn increasing attention due to their potential in wearable electronics for body-motion monitoring, human-machine interfaces, etc. However, current pressure sensors are usually assembled with polymer substrates or encapsulation layers, thus causing discomfort during wearing (i.e., low air/vapor permeability, mechanical mismatch) and restricting their applications. A breathable and flexible pressure sensor is reported with nonwoven fabrics as both the electrode (printed with MXene interdigitated electrode) and sensing (coated with MXene/silver nanowires) layers via a scalable screen-printing approach. Benefiting from the multi-layered porous structure, the sensor demonstrates good air permeability with high sensitivity (770.86–1434.89 kPa⁻¹), a wide sensing range (0–100 kPa), fast response/recovery time (70/81 ms), and low detection limit (≈1 Pa). Particularly, this sensor can detect full-scale human motion (i.e., small-scale pulse beating and large-scale walking/running) with high sensitivity, excellent cycling stability, and puncture resistance. Additionally, the sensing layer of the pressure sensor also displays superior sensitivity to humidity changes, which is verified by successfully monitoring human breathing and spoken words while wearing a sensor-embedded mask. Given the outstanding features, this breathable sensor shows promise in the wearable electronic field for body health monitoring, sports activity detection, and disease diagnosis.     

Piezoelectric sensor based on electrospun PVDF-MWCNT-Cloisite 30B hybrid nanocomposites

Piezoelectric materials have attracted substantial interest in applications such as sensors and actuators. Ferroelectric and piezoelectric polymeric fibers doped with nanoparticles are made for use in nanoscale electronic devices. In this paper, we report on poly (vinylidene fluoride) (PVDF) nanocomposites doped with different ratios of multi-walled carbon nanotube (MWCNT) and Cloisite 30B (OMMT) nanoclay prepared by electrospinning technique. The effect of different ratios of OMMT and MWCNT nanofillers and potential synergistic effect of these fillers on the crystalline structure of PVDF and the performance of resulting piezo-device were studied. Results showed that OMMT increases beta phase crystals and piezoelectric properties of PVDF as compared with MWCNT. Meanwhile, MWCNT decreases impedance and increases dielectric constant of PVDF as compared with OMMT. The acoustic absorption behavior of PVDF/MWCNT/OMMT hybrid nanocomposite was also investigated. It was found that the sound absorption efficiency of PVDF/MWCNT/OMMT hybrid nanocomposites was increased compared with that of pure PVDF fibers and film. No synergistic effect of OMMT and MWCNT on the properties of PVDF was observed.     

Inkjet Printing of Latex‐Based High‐Energy Microcapacitors

Microenergy storage devices are appealing and highly demanded for diverse miniaturized electronic devices, ranging from microelectromechanical system, robotics, to sensing microsystems and wearable electronics. However, making high‐energy microcapacitors with currently available printing technologies remains challenging. Herein, the possibility to use latex polyvinylidene fluoride (PVDF) as aqueous ink for making dielectric capacitors at the microscale is shown. The dielectric properties of printed microcapacitors can be optimized based on a novel approach, i.e., mixing PVDF latex with polyvinyl alcohol (PVA) to realize dielectric organic nanocomposites. The PVA prevents the coalescence of PVDF nanoparticles and serves as a continuous matrix phase with high dielectric breakdown strength. While the well‐dispersed PVDF nanoparticles serve as highly polarizable and isolated domains, providing large electric displacement under high fields. Consequently, a high discharged energy density of 12 J cm^?3 is achieved at 550 MV m^?1. These printed microcapacitors demonstrate mechanical robustness and dielectric stability over time.     

Ultra-High Toughness Fibers Using Controlled Disorder of Assembled Aramid Nanofibers

Assembling nanoscale building blocks with reduced defects has emerged as a promising approach to exploit nanomaterials in the fabrication of simultaneously strong and tough architectures at larger scales. Aramid nanofibers (ANFs), a type of organic nanobuilding block, have been spotlighted due to their superior mechanical properties and thermal stability. However, no breakthrough research has been conducted on the high mechanical properties of a structure composed of ANFs. Here, assembling ANFs into macroscale fiber using a simultaneous protonation and wet-spinning process is studied to reduce defects and control disorder. The ANF-assembled fibers consist of hierarchically aligned nanofibers that behave as a defective law structure, making it possible to reach a Young's modulus of 53.15 ± 8.98 GPa, a tensile strength of 1,353.64 ± 92.98 MPa, and toughness of 128.66 ± 14.13 MJ m⁻³. Compared to commercial aramid fibers, the fibers exhibit ≈1.6 times greater toughness while also providing specific energy to break as 93 J g⁻¹. Furthermore, this shows recyclability of the ANF assembly by retaining ≈94% of the initial mechanical properties. This study demonstrates a facile process to produce high stiffness and strength fibers composed of ANFs that possess significantly greater toughness than commercial synthetic fibers.     

Highly Flexible Organic Nanofiber Phototransistors Fabricated on a Textile Composite for Wearable Photosensors

Highly flexible organic nanofiber phototransistors are fabricated on a highly flexible poly(ethylene terephthalate) (PET) textile/poly(dimethylsiloxane) (PDMS) composite substrate. Organic nanofibers are obtained by electrospinning, using a mixture of poly(3,3^″′‐didodecylquarterthiophene) (PQT‐12) and poly(ethylene oxide) (PEO) as the semiconducting polymer and processing aid, respectively. PDMS is used as both a buffer layer for flattening the PET textile and a dielectric layer in the bottom‐gate bottom‐contact device configuration. PQT‐12:PEO nanofibers can be well‐aligned on the textile composite substrate by electrospinning onto a rotating drum collector. The nanofiber phototransistors fabricated on the PET/PDMS textile composite substrate show highly stable device performance (on‐current retention up to 82.3 (±6.7)%) under extreme bending conditions, with a bending radius down to 0.75 mm and repeated tests over 1000 cycles, while those prepared on film‐type PET and PDMS‐only substrates exhibit much poorer performances. The photoresponsive behaviors of PQT‐12:PEO nanofiber phototransistors have been investigated under light irradiation with different wavelengths. The maximum photoresponsivity, photocurrent/dark‐current ratio, and external quantum efficiency under blue light illumination were 930 mA W^?1, 2.76, and 246%, respectively. Furthermore, highly flexible 10 × 10 photosensor arrays have been fabricated which are able to detect incident photonic signals with high resolution. The flexible photosensors described herein have high potential for applications as wearable photosensors.     

Multiscale Structural Nanocellulosic Triboelectric Aerogels Induced by Hofmeister Effect

The advent of self-powered wearable electronics will revolutionize the fields of smart healthcare and sports monitoring. This technological advancement necessitates more stringent design requirements for triboelectric materials. The triboelectric aerogels must enhance their mechanical properties to address the issue of structural collapse in real-world applications. This study fabricates stiff nanocellulosic triboelectric aerogels with multiscale structures induced by the Hofmeister effect. The aggregation and crystallization of polymer molecular chains are enhanced by the Hofmeister effect, while ice crystal growth imparts a porous structure to the aerogel at the micron scale. Therefore, the triboelectric aerogel exhibits exceptional stiffness, boasting a Young's modulus of up to 142.9 MPa and a specific modulus of up to 340.6 kN m kg^–1, while remaining undeformed even after supporting 6600 times its weight. Even after withstanding an impact of 343 kPa, highly robust wearable self-powered sensors fabricated with triboelectric aerogels remain operational. Additionally, the self-powered sensor is capable of accurately detecting human movements, particularly in abnormal fall postures detection. This study provides considerable research and practical value for promoting material design and broadening application scenarios for self-powered wearable electronics.     

Multifunctional Artificial Artery from Direct 3D Printing with Built‐In Ferroelectricity and Tissue‐Matching Modulus for Real‐Time Sensing and Occlusion Monitoring

Treating vascular grafts failure requires complex surgery procedures and is associated with high risks. A real‐time monitoring vascular system enables quick and reliable identification of complications and initiates safer treatments early. Here, an electric fieldassisted 3D printing technology is developed to fabricate in situ‐poled ferroelectric artificial arteries that offer battery‐free real‐time blood pressure sensing and occlusion monitoring capability. The functional artery architecture is made possible by the development of a ferroelectric biocomposite which can be quickly polarized during printing and reshaped into devised objects. The synergistic effect from the potassium sodium niobite particles and the polyvinylidene fluoride polymer matrix yields a superb piezoelectric performance (bulk‐scale d₃₃ > 12 pC N^?1). The sinusoidal architecture brings the mechanical modulus close to the level of blood vessels. The desired piezoelectric and mechanical properties of the artificial artery provide an excellent sensitivity to pressure change (0.306 mV mmHg^?1, R² > 0.99) within the range of human blood pressure (11.25–225.00 mmHg). The high pressure sensitivity and the ability to detect subtle vessel motion pattern change enable early detection of partial occlusion (e.g., thrombosis), allowing for preventing grafts failure. This work demonstrates a promising strategy of incorporating multifunctionality to artificial biological systems for smart healthcare systems.