Reversible Molecule Interactions Enable Ultrastretchable and Recyclable Ionogels for Wearable Piezoionic Sensors.

Ionogel-based piezoionic sensors feel motions and strains like human skin relying on reversible ion migrations under external mechanical stimulus and are of great importance to artificial intelligence. However, conventional ion-conductive polymers behave with degraded electrical and mechanical properties after thousands of strain cycles, and the discarded materials and devices become electronic wastes as well. Here, we develop ultrastretchable ionogels with superior electrical properties via the mediation of metal-organic frameworks, whose properties are attributed to reversible molecule interactions inside the material system. Ionogels present excellent mechanical properties with breaking elongation as high as 850%, exceeding most previously reported similar materials, and the high conductivity enables further application in sensor devices. In addition, our ionogels display superior recyclability because of the reversible physical and chemical interactions inside material molecules, which are eco-friendly to the environment. As a result, the ionogel-based piezoionic sensors deliver high sensitivity, flexibility, cyclic stability, and signal reliability, which are of great significance to wearable applications in human-motion detections such as throat vibration, facial expression, joint mobility, and finger movement. Our study paves the way for ultrastretchable and eco-friendly ionogel design for flexible electrochemical devices.

Air-Writing Recognition Enabled by a Flexible Dual-Network Hydrogel-Based Sensor and Machine Learning.

Accurate air-writing recognition is pivotal for advancing state-of-the-art text recognizers, encryption tools, and biometric technologies. However, most existing air-writing recognition systems rely on image-based sensors to track hand and finger motion trajectories. Additionally, users' writing is often guided by delimiters and imaginary axes which restrict natural writing movements. Consequently, recognition accuracy falls short of optimal levels, hindering performance and usability for practical applications. Herein, we have developed an approach utilizing a one-dimensional convolutional neural network (1D-CNN) algorithm coupled with an ionic conductive flexible strain sensor based on a sodium chloride/sodium alginate/polyacrylamide (NaCl/SA/PAM) dual-network hydrogel for intelligent and accurate air-writing recognition. Taking advantage of the excellent characteristics of the hydrogel sensor, such as high stretchability, good tensile strength, high conductivity, strong adhesion, and high strain sensitivity, alongside the enhanced analytical ability of the 1D-CNN machine learning (ML) algorithm, we achieved a recognition accuracy of ∼96.3% for in-air handwritten characters of the English alphabets. Furthermore, comparative analysis against state-of-the-art methods, such as the widely used residual neural network (ResNet) algorithm, demonstrates the competitive performance of our integrated air-writing recognition system. The developed air-writing recognition system shows significant potential in advancing innovative systems for air-writing recognition and paving the way for exciting developments in human-machine interface (HMI) applications.

3D Stretchable Electronics with Stretchable Interlayer Connectors.

The unique mechanical characteristics of stretchable electronics has significantly expanded applications by overcoming the limitations (rigid, planar) of conventional electronics. However, most reported stretchable electronics are two dimensionally stretchable (laterally stretchable in the xy-axis) in a single layer or even in multiple layers. In this report, we present three dimensionally (3D) stretchable electronics (laterally and vertically stretchable in the xyz-axes) in multilayered 3D electronic circuits. Computational and experimental studies indicate that the approach is reliable in three-dimensional deformations. The base units, stretchable interlayer connectors, can be applied to form various electronic circuit designs in 3D stretchable forms. We demonstrated the efficacy of the approach by designing and fabricating a 3D stretchable light emitting diode (LED) matrix display (125 LEDs).

Stretchable Heat Transfer Eco-Materials: Mesogen Grafted NR-Based Nanocomposites with High Thermal Conductivity and Low Dielectric Constant.

Biomass-based functional polymers have received significant attention across various fields, in view of eco-friendly human society and sustainable growth. In this context, there are efforts to functionalize the biomass polymers for next-generation polymer materials. Here, stretchable heat transfer materials are focused on which are essential for stretchable electronics and future robotics. To achieve this goal, natural rubber (NR) is chemically modified with a thiol-terminated phenylnaphthalene (TTP), and then utilized as a thermally conductive NR (TCNR) matrix. Hexagonal boron nitride (h-BN), renowned for its high thermal conductivity and low electrical conductivity, is incorporated as a filler to develop stretchable heat transfer eco-materials. The optimized TCNR/h-BN composite elongates to 140% due to great elasticity of NR, and exhibits excellent dielectric properties (a low dielectric constant of 2.26 and a low dielectric loss of 0.006). Furthermore, synergetic phonon transfer of phenylnaphthalene crystallites and h-BN particles in the composite results in a high thermal conductivity of 0.87 W m-1 K-1. The outstanding thermal, mechanical, and dielectric properties of the newly developed TCNR/h-BN composite enable the successful demonstration as stretchable and shape-adaptable thermal management materials.

Toward Integrated Multifunctional Laser-Induced Graphene-Based Skin-Like Flexible Sensor Systems.

The burgeoning demands for health care and human-machine interfaces call for the next generation of multifunctional integrated sensor systems with facile fabrication processes and reliable performances. Laser-induced graphene (LIG) with highly tunable physical and chemical characteristics plays vital roles in developing versatile skin-like flexible or stretchable sensor systems. This Progress Report presents an in-depth overview of the latest advances in LIG-based techniques in the applications of flexible sensors. First, the merits of the LIG technique are highlighted especially as the building blocks for flexible sensors, followed by the description of various fabrication methods of LIG and its variants. Then, the focus is moved to diverse LIG-based flexible sensors, including physical sensors, chemical sensors, and electrophysiological sensors. Mechanisms and advantages of LIG in these scenarios are described in detail. Furthermore, various representative paradigms of integrated LIG-based sensor systems are presented to show the capabilities of LIG technique for multipurpose applications. The signal cross-talk issues are discussed with possible strategies. The LIG technology with versatile functionalities coupled with other fabrication strategies will enable high-performance integrated sensor systems for next-generation skin electronics.

Stretchable Metamaterials with Tunable Infrared Emissivity for Dynamic Thermal Management.

Manipulation of infrared emissivity, which is closely related to surface structure and optical parameters of materials, is a crucial approach for realizing dynamic thermal management. In this study, we design a metamaterial consisting of an array of aluminum disks embedded on a surface of a stretchable elastomeric substrate. Mechanical stretching-induced deformation allows dynamic modification of the surface structure and equivalent optical parameters, thus enabling dynamic control of the emissivity. By utilizing the elastomer polydimethylsiloxane (PDMS) as the substrate, the microstructure interdisk gap can be altered by stretching the PDMS. Through theoretical calculations, the plausibility of this approach is explained by the excitation of plasmon resonance and the variation in the exposed area of highly absorbent PDMS, and the optimal structures for tuning the infrared emissivity are revealed to be 6 µm in diameter and 100 nm in height. Based on this design, we prepare samples with periods of 7 and 7.9 µm and experimentally demonstrate that a change in the period can cause a change in the emissivity and thus tunability in thermal control performance. The temperature difference between the two samples reaches 44.1 °C at a heating power of 0.28 W/cm2 for both samples. Furthermore, we construct a stretching platform that enables in situ mechanical stretching to realize dynamic changes in emissivity. The integral infrared emissivity of the sample increases from 0.32 to 0.5 at a biaxial tensile strain of 13%, achieving a 56% modulation rate of the integral infrared emissivity. The material is expected to enable dynamic thermal management.

Stretchable and Elastic Triboelectric Nanogenerator with Liquid-Metal Grid-Patterned Single Electrode for Wearable Energy-Harvesting Devices.

Triboelectric nanogenerators (TENGs) have garnered significant attention as efficient energy-harvesting systems for sustainable energy sources in the field of self-powered wearable devices. Various conductive materials are used to build wearable devices, among which, gallium-based liquid metal (LM) is a preferred electrode owing to its fluidity and metallic conductivity even when strained. In this study, a stretchable, elastic, and wearable triboelectric nanogenerator is designed using a single electrode fabricated by embedding LM grid patterns into a stretchable silicone substrate through a two-step spray-coating process. Contrary to conventional double-electrode TENG that is challenging to integrate to human body, the LM grid-patterned single-electrode TENG (LMG-SETENG) has a simplified design and provides more flexibility. The LMG-SETENG can generate voltages of up to 100 V via triboelectrification upon contact with the human body, even under various degrees of strain, owing to the fluidity of the LM electrode. The generated energy can be utilized as a sustainable energy source to power various small appliances. Moreover, the proposed LMG-SETENG can be utilized in soft robotics, electronic skin, and healthcare devices.

High-Performance Stretchable Strain Sensors Based on Auxetic Fabrics for Human Motion Detection.

Wearable strain sensors play a pivotal role in real-time human motion detection and health monitoring. Traditional fabric-based strain sensors, typically with a positive Poisson's ratio, face challenges in maintaining sensitivity and comfort during human motion due to conflicting resistance changes in different strain directions. In this work, high-performance stretchable strain sensors are developed based on graphene-modified auxetic fabrics (GMAF) for human motion detection in smart wearable devices. The proposed GMAF sensors, with a negative Poisson's ratio achieved through commercially available warp-knitting technology, exhibit an 8-fold improvement in sensitivity compared to conventional plain fabric sensors. The unique auxetic fabric structure enhances sensitivity by synchronizing resistance changes in both wale and course directions. The GMAF sensors demonstrate excellent washability, showing only slight degradation in auxeticity and an acceptable increase in resistance after 10 standard wash cycles. The GMAF sensors maintain stability under different strain levels and various motion frequencies, emphasizing their dynamic performance. The sensors exhibit superior conformability to joint movements, which effectively monitor a full range of motions, including joint bending, sports activities, and subtle actions like coughing and swallowing. The research underscores a promising approach to achieve industrial-scale production of wearable sensors with improved performance and comfort through fabric structure design.

Development of a Highly Sensitive and Stretchable Charge-Transfer Fiber Strain Sensor for Wearable Applications.

Wearable electronics have significantly advanced the development of highly stretchable strain sensors, which are essential for applications such as health monitoring, human-machine interfaces, and energy harvesting. Fiber-based sensors and polymeric materials are promising due to their flexibility and tunable properties, although balancing sensitivity and stretchability remains a challenge. This study introduces a novel composite strain sensor that combines poly(3-hexylthiophene) and tetrafluoro-tetracyanoquinodimethane to form a charge-transfer complex (CTC) with carbon nanotubes (CNTs) on a styrene-butadiene-styrene substrate. The CTC improves conductivity through effective charge transfer, while CNTs provide mechanical reinforcement and maintain conductive paths, preventing cracks under large strains. Purposefully introduced wrinkles in the structure enhance the detection of small strains. The sensor demonstrated a broad strain-sensing range from 0.01 to 200%, exhibiting high sensitivity to both minor and major deformations. Mechanical tests confirmed strong stress-strain performance, and electrical tests indicated significant conductivity improvements with CNT integration. These results highlight the potential of the sensor for applications in health monitoring, human-machine interfaces, and energy harvesting, effectively mimicking the tactile sensing abilities of human skin.

Durable Flexible Conductive Fiber Based on Cross-Linking Network Tannic Acid/Polypyrrole for Wearable Thermotherapy Monitoring System.

Intelligent wearable textiles have garnered attention and advancement, particularly in the realms of thermotherapy and health monitoring. As a critical component of intelligent wearable textiles, conductive fibers are expected to have long-term stable and durable conductivity. In this work, a highly stretchable and conductive fiber based on tannic acid/polypyrrole was developed. The conductive network was formed by doping TA into PPy, resulting in enhanced stretchability of PPy on the surface of PU. TA also improves the interface interaction between PPy and PU to gain more firm attachment of PPy, which achieves high conductivity (0.89 ± 0.23 S/cm) and durability. Furthermore, the stretchable conductive fiber also exhibited intelligent responses to electricity, light, and deformation. They can serve as heat sources under the action of electricity and light (temperature was raised to 42 °C under 4 V and 54 °C under solar radiation stimuli) and can also monitor the movements of humans, making them potential applications in thermotherapy textiles and intelligent sensing equipment. A PU/TA/PPy-based all-in-one smart wearable system was fabricated using textile molding technology capable of all-weather thermal therapy and motion detection. This fiber fabrication technology and integrated system offer insights for the future development of smart wearable devices.

Stretchable and Self-Cleaning Daytime Radiative Coolers for Human Fabric and Building Applications.

Advancements in radiative cooling technology have shown significant progress in recent years. However, the limited mechanical properties of most radiative coolers greatly hinder their practical applications, particularly in the context of human cooling fabrics. In this study, we present the fabrication of facile and stretchable radiative coolers with exceptional cooling performance by utilizing the design of porous radiative coolers as guidelines for developing promising elastomer coolers. Subsequently, we employ a simple electrospinning method to fabricate these coolers, resulting in impressive solar reflectivity (∼96.1%) and infrared emissivity (over 95%). During the summer, these coolers demonstrate a maximum temperature drop of ∼9.6 °C. Additionally, the developed coolers exhibit superior hydrophobicity and mechanical properties, with a high strain capacity exceeding 700% and a stress tolerance of over 30 MPa, highlighting their potential for application in automobile textiles and cooling fabrics. Furthermore, we evaluate the radiative cooling performance of stretchable coolers using global-scale modeling, revealing their significant cooling potential across various regions worldwide.

Jellyfish-like Gold Nanowires as FlexoSERS Sensors for Sweat Analysis.

We introduce the FlexoSERS sensor, which is notable for its high stretchability, sensitivity, and patternability. Featuring a hierarchically oriented jellyfish-like architecture constructed from stretchable gold nanowires, this sensor provides an ultrasensitive SERS signal even under 50% strain, with an enhancement factor (EF) of 3.3 × 1010. Impressively, this heightened performance remains consistently robust across 2,500 stretch-release cycles. The integration of nanowires with 3D-printed hydrogel enables a customizable FlexoSERS sensor, facilitating localized sweat collection and detection. The FlexoSERS sensor successfully detects and quantifies uric acid (UA) in both artificial and human sweat and functions as a pH sensor with repeatability and sensitivity across a pH range of 4.2-7.8, enabling real-time sweat monitoring during exercise. In summary, the rational architectural design, scalable fabrication process, and hydrogel integration collectively position this nanowire-based FlexoSERS sensor as a highly promising platform for customizable wearable sweat diagnostics.

Highly Stretchable, Tissue-like Ag Nanowire-Enhanced Ionogel Nanocomposites as an Ionogel-Based Wearable Sensor for Body Motion Monitoring.

The development of wearable electronic devices for human health monitoring requires materials with high mechanical performance and sensitivity. In this study, we present a novel transparent tissue-like ionogel-based wearable sensor based on silver nanowire-reinforced ionogel nanocomposites, P(AAm-co-AA) ionogel-Ag NWs composite. The composite exhibits a high stretchability of 605% strain and a moderate fracture stress of about 377 kPa. The sensor also demonstrates a sensitive response to temperature changes and electrostatic adsorption. By encapsulating the nanocomposite in a polyurethane transparent film dressing, we address issues such as skin irritation and enable multidirectional stretching. Measuring resistive changes of the ionogel nanocomposite in response to corresponding strain changes enables its utility as a highly stretchable wearable sensor with excellent performance in sensitivity, stability, and repeatability. The fabricated pressure sensor array exhibits great proficiency in stress distribution, capacitance sensing, and discernment of fluctuations in both external electric fields and stress. Our findings suggest that this material holds promise for applications in wearable and flexible strain sensors, temperature sensors, pressure sensors, and actuators.

Highly Conductive and Stretchable Hydrogel Nanocomposite Using Whiskered Gold Nanosheets for Soft Bioelectronics.

The low electrical conductivity of conductive hydrogels limits their applications as soft conductors in bioelectronics. This low conductivity originates from the high water content of hydrogels, which impedes facile carrier transport between conductive fillers. This study presents a highly conductive and stretchable hydrogel nanocomposite comprising whiskered gold nanosheets. A dry network of whiskered gold nanosheets is fabricated and then incorporated into the wet hydrogel matrices. The whiskered gold nanosheets preserve their tight interconnection in hydrogels despite the high water content, providing a high-quality percolation network even under stretched states. Regardless of the type of hydrogel matrix, the gold-hydrogel nanocomposites exhibit a conductivity of ≈520 S cm-1 and a stretchability of ≈300% without requiring a dehydration process. The conductivity reaches a maximum of ≈3304 S cm-1 when the density of the dry gold network is controlled. A gold-adhesive hydrogel nanocomposite, which can achieve conformal adhesion to moving organ surfaces, is fabricated for bioelectronics demonstrations. The adhesive hydrogel electrode outperforms elastomer-based electrodes in in vivo epicardial electrogram recording, epicardial pacing, and sciatic nerve stimulation.

Stretchable Triboelectric Nanogenerator Based on Liquid Metal with Varying Phases.

Stretchable triboelectric nanogenerators (TENGs) represent a new class of energy-harvesting devices for powering wearable devices. However, most of them are associated with poor stretchability, low stability, and limited substrate material choices. This work presents the design and demonstration of highly stretchable and stable TENGs based on liquid metalel ectrodes with different phases. The conductive and fluidic properties of eutectic gallium-indium (EGaIn) in the serpentine microfluidic channel ensure the robust performance of the EGaIn-based TENG upon stretching over several hundred percent. The bi-phasic EGaIn (bGaIn) from oxidation lowers surface tension and increases adhesion for printing on diverse substrates with high output performance parameters. The optimization of the electrode shapes in the bGaIn-based TENGs can reduce the device footprint and weight, while enhancing stretchability. The applications of the EGaIn- and bGaIn-based TENG include smart elastic bands for human movement monitoring and smart carpets with integrated data transmission/processing modules for headcount monitoring/control. Combining the concept of origami in the paper-based bGaIn TENG can reduce the device footprint to improve output performance per unit area. The integration of bGaIn-TENG on a self-healing polymer substrate with corrosion resistance against acidic and alkaline solutions further facilitates its use in various challenging and extreme environments.

Materials, Structure, and Interface of Stretchable Interconnects for Wearable Bioelectronics.

Since wearable technologies for telemedicine have emerged to tackle global health concerns, the demand for well-attested wearable healthcare devices with high user comfort also arises. Skin-wearables for health monitoring require mechanical flexibility and stretchability for not only high compatibility with the skin's dynamic nature but also a robust collection of fine health signals from within. Stretchable electrical interconnects, which determine the device's overall integrity, are one of the fundamental units being understated in wearable bioelectronics. In this review, a broad class of materials and engineering methodologies recently researched and developed are presented, and their respective attributes, limitations, and opportunities in designing stretchable interconnects for wearable bioelectronics are offered. Specifically, the electrical and mechanical characteristics of various materials (metals, polymers, carbons, and their composites) are highlighted, along with their compatibility with diverse geometric configurations. Detailed insights into fabrication techniques that are compatible with soft substrates are also provided. Importantly, successful examples of establishing reliable interfacial connections between soft and rigid elements using novel interconnects are reviewed. Lastly, some perspectives and prospects of remaining research challenges and potential pathways for practical utilization of interconnects in wearables are laid out.

High-Performance Intrinsically Stretchable Organic Photovoltaics Enabled by Robust Silver Nanowires/S-PH1000 Hybrid Transparent Electrodes.

Intrinsically stretchable organic photovoltaics (is-OPVs) hold significant promise for integration into self-powered wearable electronics. However, their potential is hindered by the lack of sufficient consistency between optoelectronic and mechanical properties. This is primarily due to the limited availability of stretchable transparent electrodes (STEs) that possess both high conductivity and stretchability. Here, a hybrid STE with exceptional conductivity, stretchability, and thermal stability is presented. Specifically, STEs are composed of the modified PH1000 (referred to as S-PH1000) and silver nanowires (AgNWs). The S-PH1000 endows the STE with good stretchability and smoothens the surface, while the AgNWs enhance the charge transport. The resulting hybrid STEs enable is-OPVs to a remarkable power conversion efficiency (PCE) of 16.32%, positioning them among the top-performing is-OPVs. With 10% elastomer, the devices retain 82% of the initial PCE after 500 cycles at 20% strain. Additionally, OPVs equipped with these STEs exhibit superior thermal stability compared to those using indium tin oxide electrodes, maintaining 75% of the initial PCE after annealing at 85 °C for 390 h. The findings underscore the suitability of the designed hybrid electrodes for efficient and stable is-OPVs, offering a promising avenue for the future application of OPVs.

Liquid Metal-Based Self-Healing Conductors for Flexible and Stretchable Electronics.

Flexible and stretchable electronics rely on compliant conductors as essential building materials. However, these materials are susceptible to wear and tear, leading to degradation over time. In response to this concern, self-healing conductors have been developed to prolong the lifespan of functional devices. These conductors can autonomously restore their properties following damage. Conventional self-healing conductors typically comprise solid conductive fillers and healing agents dispersed within polymer matrices. However, the solid additives increase the stiffness and reduce the stretchability of the resulting composites. There is growing interest in utilizing gallium-based liquid metal alloys due to their exceptional electrical conductivity and liquid-phase deformability. These liquid metals are considered attractive candidates for developing compliant conductors capable of automatic recovery. This perspective delves into the rapidly advancing field of liquid metal-based self-healing conductors, exploring their design, fabrication, and critical applications. Furthermore, this article also addresses the current challenges and future directions in this active area of research.

Highly Adhesive and Stretchable Epidermal Electrode for Bimodal Recording Patch.

For numerous biological and human-machine applications, it is critical to have a stable electrophysiological interface to obtain reliable signals. To achieve this, epidermal electrodes should possess conductivity, stretchability, and adhesiveness. However, limited types of materials can simultaneously satisfy these requirements to provide satisfying recording performance. Here, we present a dry electromyography (EMG) electrode based on conductive polymers and tea polyphenol (CPT), which offers adhesiveness (0.51 N/cm), stretchability (157%), and low impedance (14 kΩ cm2 at 100 Hz). The adhesiveness of the electrode is attributed to the interaction between catechol groups and hydroxyls in the polymer blend. This adhesive electrode ensures stable EMG recording even in the presence of vibrations and provides signals with a high signal-to-noise ratio (>25 dB) for over 72 h. By integrating the CPT electrode with a liquid metal strain sensor, we have developed a bimodal rehabilitation monitoring patch (BRMP) for sports injuries. The patch utilizes Kinesio Tape as a substrate, which serves to accelerate rehabilitation. It also tackles the challenge of recording with knee braces by fitting snugly between the brace and the skin, due to its thin and stretchable design. CPT electrodes not only enable BRMP to assist clinicians in formulating effective rehabilitation plans and offer patients a more comfortable rehabilitation experience, but also hold promise for future applications in biological and human-machine interface domains.

Simulation-Guided Analysis towards Trench Depth Optimization for Enhanced Flexibility in Stretch-Free, Shape-Induced Interconnects for Flexible Electronics.

In this paper, we present an optimization of the planar manufacturing scheme for stretch-free, shape-induced metal interconnects to simplify fabrication with the aim of maximizing the flexibility in a structure regarding stress and strain. The formation of trenches between silicon islands is actively used in the lithographic process to create arc shape structures by spin coating resists into the trenches. The resulting resist form is used as a template for the metal lines, which are structured on top. Because this arc shape is beneficial for the flexibility of these bridges. The trench depth as a key parameter for the stress distribution is investigated by applying numerical simulations. The simulated results show that the increase in penetration depth of the metal bridge into the trench increases the tensile load which is converted into a shear force Q(x), that usually leads to increased strains the structure can generate. For the fabrication, the filling of the trenches with resists is optimized by varying the spin speed. Compared to theoretical resistance, the current-voltage measurements of the metal bridges show a similar behavior and almost every structural variation is capable of functioning as a flexible electrical interconnect in a complete island-bridge array.