Superhydrophobic, Anti-Freezing and Multi-Cross-Linked Wearable Hydrogel Strain Sensor for Underwater Gesture Recognition.

Conductive hydrogel is considered to be one of the most potential sensing materials for wearable strain sensors. However, both the hydrophilicity of polymer chains and high water content severely inhibit the potential applications of hydrogel-based sensors in extreme conditions. In this study, a multicross-linked hydrogel was prepared by simultaneously introducing a double-network matrix, multiple conductive fillers, and free-moving ions, which can withstand an ultralow temperature below -80 °C. A superhydrophobic Ecoflex layer with a water contact angle of 159.1° was coated on the hydrogel using simple spraying and laser engraving methods. Additionally, the smart glove integrating five hydrogel strain sensors with a microprocessor was developed to recognize 12 types of diving gestures and synchronously transmit recognition results to smartphones. The superhydrophobic and antifreezing hydrogel strain sensor proposed in this study emerges promising potentials in wearable electronics, human-machine interfaces, and underwater applications.

Ultra-Stretchable Composite Organohydrogels Polymerized Based on MXene@Tannic Acid-Ag Autocatalytic System for Highly Sensitive Wearable Sensors.

Conductive hydrogels have attracted widespread attention in the fields of biomedicine and health monitoring. However, their practical application is severely hindered by the lengthy and energy-intensive polymerization process and weak mechanical properties. Here, a rapid polymerization method of polyacrylic acid/gelatin double-network organohydrogel is designed by integrating tannic acid (TA) and Ag nanoparticles on conductive MXene nanosheets as catalyst in a binary solvent of water and glycerol, requiring no external energy input. The synergistic effect of TA and Ag NPs maintains the dynamic redox activity of phenol and quinone within the system, enhancing the efficiency of ammonium persulfate to generate radicals, leading to polymerization within 10 min. Also, ternary composite MXene@TA-Ag can act as conductive agents, enhanced fillers, adhesion promoters, and antibacterial agents of organohydrogels, granting them excellent multi-functionality. The organohydrogels exhibit excellent stretchability (1740%) and high tensile strength (184 kPa). The strain sensors based on the organohydrogels exhibit ultrahigh sensitivity (GF = 3.86), low detection limit (0.1%), and excellent stability (>1000 cycles, >7 days). These sensors can monitor the human limb movements, respiratory and vocal cord vibration, as well as various levels of arteries. Therefore, this organohydrogel holds potential for applications in fields such as human health monitoring and speech recognition.

Mechanically Durable Superhydrophobic Strain Sensors with High Biocompatibility and Sensing Performance for Underwater Motion Monitoring.

Much progress has been made toward the development of wearable flexible strain sensors with high sensing performance to monitor human motion, but continuous function in harsh aqueous environments remains a significant challenge. A promising strategy has been the design of sensors with highly durable superhydrophobicity and maintenance of unique sensing properties. Herein, an extremely durable superhydrophobic strain sensor with an ultrawide sensing range was simply fabricated by directly brushing conductive carbon black nanoparticles (CBNPs) onto an elastic silicone rubber sheet (SS) with poly(dimethylsiloxane) (PDMS) coatings (i.e., SS/PDMS-CBNPs sensors). First, this method avoided the use of toxic solvents and a conventional prestretching treatment. Second, considering the easily destroyed rough structures and surface chemistry for conventional superhydrophobic sensors during practical applications, the prepared SS/PDMS-CBNP sensors showed excellent mechanical durability of both superhydrophobicity and sensing as examined by harsh abrasion (300 cycles), stretching (up to 200%), and ultrasonication (40 min) treatments. Third, the prepared superhydrophobic strain sensor exhibited high sensitivity (gauge factor of 101.75), high stretchability (0.015-460%), low hysteresis (83 ms), and long-term stability (10000 cycles). Fourth, the high biocompatibility of the SS/PDMS-CBNP sensor was demonstrated by rabbit skin irritation tests. Finally, the remarkable water-repellent and sensing properties of the SS/PDMS-CBNP sensor allowed its application to monitor a swimmer's real-time situation and send distress signals when needed.

Highly Conductive and Sensitive Wearable Strain Sensors with Metal/Nanoparticle Double Layer for Noninterference Voice Detection.

Human voice recognition via skin-attachable devices has significant potential for gathering important physiological information from acoustic data without background noise interference. In this study, a highly sensitive and conductive wearable crack-based strain sensor was developed for voice-recognition systems. The sensor was fabricated using a double-layer structure of Ag nanoparticles (NPs) and Ag metal on a biocompatible polydimethylsiloxane substrate. The top metal layer acts as a conducting active layer, whereas the bottom Ag NP layer induces channel cracks in the upper layer, effectively hindering current flow. Subsequently, the double-layer film exhibits a low electrical resistance value (<5 × 10-5 Ω cm), ultrahigh sensitivity (gauge factor = 1870), and a fast response/recovery time (252/168 µs). A sound wave was detected at a high frequency of 15 kHz with a signal-to-noise ratio (SNR) over 40 dB. The sensor exhibited excellent anti-interference characteristics and effectively differentiated between different voice qualities (modal, pressed, and breathy), with a systematic analysis revealing successful detection of the laryngeal state and glottal source. This ultrasensitive wearable sensor has potential applications in various physiological signal measurement methods, personalized healthcare systems, and ubiquitous computing.

Breathable and Wearable Strain Sensors Based on Synergistic Conductive Carbon Nanotubes/Cotton Fabrics for Multi-directional Motion Detection.

Flexible strain-sensitive sensors have been receiving intensive attention in many aspects ranging from human motion capture to health-related signal monitoring. However, the fabric strain sensor with multi-directional sensing capability, besides having a wide strain range and high response sensitivity, is still very challenging and deserves further exploration. Here, we have prepared a wearable cotton fabric strain sensor uniformly decorated with single-walled carbon nanotubes through a facile solution process. The unique hierarchical architecture of the cotton fabric woven from twisted yarns combined with the conductive carbon nanotube network endows the fabric strain sensors with attractive performance, including low detection limit, large workable strain range, fascinating stability and durability, excellent direction-dependent strain response, and good air permeability. The strain sensor without polymer encapsulation can not only monitor subtle and large multi-directional motions but also fit well to the human body with satisfactory comfort, demonstrating its potential application in wearable electronics and intelligent clothing.

Ultra-stretchable, super-hydrophobic and high-conductive composite for wearable strain sensors with high sensitivity.

With continuous development of artificial intelligence technology, strain sensors have attracted widespread attention. In this work, a novel high-performance wearable strain sensor is prepared by using a kind of ultra-stretchable, super-hydrophobic and high-conductive composite. The preparation process is as follows, i.e., using common elastic band (EB) as the polymer matrix, nano carbon black (CB) and carbon nanotubes (CNTs) as mixed conductive filler, and then modified by polydimethylsiloxane (PDMS) to obtain the PDMS/(CB + CNTs)/EB composite for assembling assemble flexible wearable strain sensors. Experimental results reveal the following excellent properties: 1) The composite exhibits excellent mechanical properties and super-hydrophobicity, i.e., the tensile strength is up to 996.5%, and the elastic modulus and tensile strength increase 49.2% and 59.2%, compared with pristine EB; 2) The composite strain sensor exhibits high sensitivity (the gauge factor reaches up to 648.83 under strain range of 979.9-996.5%), and it still shows stable performance after 3000 cycles tests (100% strain); 3) It is a well candidate to be used for monitoring human body motions including large and subtle body movements; 4) The composite sensor also has advantages of easy access of raw materials, simple preparation, easy mass production and relatively low production cost, showing a broad application prospect in wearable electronic products.

Stretchable, Environment-Stable, and Knittable Ionic Conducting Fibers Based on Metallogels for Wearable Wide-Range and Durable Strain Sensors.

The construction of fibrous ionic conductors and sensors with large stretchability, low-temperature tolerance, and environmental stability is highly desired for practical wearable devices yet is challenging. Herein, metallogels (MOGs) with a rapidly reversible force-stimulated sol-gel transition were employed and encapsulated into a hollow thermoplastic elastomer (TPE) microfiber through a simple coaxial spinning. The resultant MOG@TPE coaxial fiber exhibited a high stretchability (>100%) in a broad temperature range (-50 to 50 °C). The MOG@TPE fibrous strain sensor demonstrated a high-yet-linear working curve, fast response time (<100 ms), highly stable conductivity under large deformation, and excellent cycling stability (>3000 cycles). The MOG@TPE fibrous sensors were demonstrated to be directly attached to the human skin to monitor the real-time movements of large/facet joints of the elbow, wrist, finger, and knee. It is believed that the present work for preparing the stretchable ionic conductive fibers holds great promise for applications in fibrous wearable sensors with broad temperature range, large stretchability, stable conductivity, and high wearing comfort.

Ultrasoft and Ultrastretchable Wearable Strain Sensors with Anisotropic Conductivity Enabled by Liquid Metal Fillers.

Herein, ultrasoft and ultrastretchable wearable strain sensors enabled by liquid metal fillers in an elastic polymer are described. The wearable strain sensors that can change the effective resistance upon strains are prepared by mixing silicone elastomer with liquid metal (EGaIn, Eutectic gallium-indium alloy) fillers. While the silicone is mixed with the liquid metal by shear mixing, the liquid metal is rendered into small droplets stabilized by an oxide, resulting in a non-conductive liquid metal elastomer. To attain electrical conductivity, localized mechanical pressure is applied using a stylus onto the thermally cured elastomer, resulting in the formation of a handwritten conductive trace by rupturing the oxide layer of the liquid metal droplets and subsequent percolation. Although this approach has been introduced previously, the liquid metal dispersed elastomers developed here are compelling because of their ultra-stretchable (elongation at break of 4000%) and ultrasoft (Young's modulus of <0.1 MPa) mechanical properties. The handwritten conductive trace in the elastomers can maintain metallic conductivity when strained; however, remarkably, we observed that the electrical conductivity is anisotropic upon parallel and perpendicular strains to the conductive trace. This anisotropic conductivity of the liquid metal elastomer film can manipulate the locomotion of a robot by routing the power signals between the battery and the driving motor of a robot upon parallel and perpendicular strains to the hand-written circuit. In addition, the liquid metal dispersed elastomers have a high degree of deformation and adhesion; thus, they are suitable for use as a wearable sensor for monitoring various body motions.

Low-Temperature Wearable Strain Sensor Based on a Silver Nanowires/Graphene Composite with a Near-Zero Temperature Coefficient of Resistance.

Currently, the exploration of wearable strain sensors that can work under subzero temperatures while simultaneously possessing anti-interference capability toward temperature is still a grand challenge. Herein, we present a low-temperature wearable strain sensor that is constructed via the incorporation of a Ag nanowires/graphene (Ag NWs/G) composite into the polydimethylsiloxane (PDMS) polymer. The Ag NWs/G/PDMS strain sensor exhibits promising flexibility at a very low temperature (-40 °C), outstanding fatigue resistance with low hysteresis energy, and near-zero temperature coefficient of resistance (TCR). The Ag NWs/G/PDMS strain sensor shows excellent sensing performance under subzero temperatures with a very high gauge factor of 9156 under a strain of >36%, accompanied by a noninterference characteristic to temperature (-40 to 20 °C). The Ag NWs/G/PDMS strain sensor also demonstrates the feasibility of monitoring various human movements such as finger bending, arm waving, wrist rotation, and knee bending under both room temperature and low-temperature conditions. This work initiates a new promising strategy to construct next-generation wearable strain sensors that can work stably and effectively under very low temperatures.

A mechanical, electrical dual autonomous self-healing multifunctional composite hydrogel.

The versatile properties make hydrogels a potential multipurpose material that finds wide applications. However, the preparation of multipurpose hydrogels is very challenging. Here, we report a method based on free radical reaction and composite mechanisms to prepare mechanical and electrical self-healing multifunctional hydrogels. In this study, the introduction of imidazolium salt ionic liquids and glycerol in the hydrogel system endows the gels with good antibacterial, conductive, and adhesive properties and excellent antifreeze properties. The testing results show that the as-prepared hydrogel has stable mechanical and electrical properties even under the extremely cold condition of -50°C after self-healing. Moreover, the active esters formed in the dynamic radical reaction have better reducibility, thus further investing the as-prepared hydrogel with high antioxidant activity. The application results show that these comprehensive properties make such hydrogel system very useful in wound repair and wearable strain sensors.

Highly Stretchable, Fast Self-Healing, and Waterproof Fluorinated Copolymer Ionogels with Selectively Enriched Ionic Liquids for Human-Motion Detection.

The development of waterproof ionogels with high stretchability and fast self-healing performance is essential for stretchable ionic conductors in sophisticated skin-inspired wearable sensors but can be rarely met in one material. Herein, a semicrystalline fluorinated copolymer ionogel (SFCI) with extremely high stretchability, underwater stability, and fast self-healability was fabricated, among which hydrophobic ionic liquids ([BMIM][TFSI]) were selectively enriched in fluoroacrylate segment domains of the fluorinated copolymer matrix through unique ion-dipole interactions. Benefiting from the reversible ion-dipole interactions between the [BMIM][TFSI] and fluoroacrylate segment domains as well as the physical cross-linking effects of semicrystalline oligoethylene glycol domains, the SFCI exhibited ultrastretchability (>6000%), fast room-temperature self-healability (>96% healing efficiency after cutting and self-healing for 30 min), and outstanding elasticity. In addition, the representative SFCI also exhibited high-temperature tolerance up to 300 °C, antifreezing performance as low as -35 °C, and high transparency (>93% visible-light transmittance). As a result, the as-obtained SFCI can readily be used as a highly stretchable ionic conductor in skin-inspired wearable sensors with waterproof performance for real-time detecting physiological human activities. These attractive features illustrate that the developed ultrastretchable and rapidly self-healable ionogels with unique waterproofness are promising candidates especially for sophisticated wearable strain sensing applications in complex and extreme environments.

A Biomimetic Conductive Tendril for Ultrastretchable and Integratable Electronics, Muscles, and Sensors.

Adaptive tendril coiling of climbing plants has long inspired the artificial soft microsystem for actuation and morphing. The current bionic research efforts on tendril coiling focus on either the preparation of materials with the coiling geometry or the design of self-shaping materials. However, the realization of two key functional features of the tendril, the spring-like buffering connection and the axial contraction, remains elusive. Herein, we devise a conductive tendril by fusing conductive yarns into tendril configuration, bypassing the prevailing conductivity constraints and mechanical limitations. The conductive tendril not only inherits an electrophysiology buffering mechanics with exceptional conductance retention ability against extreme stretching but also exhibits excellent contractive actuation performance. The integrative design of the ultraelastic conductive tendril shows a combination of compliant mobility, actuation, and sensory capabilities. Such smart biomimetic material holds great prospects in the fields of ultrastretchable electronics, artificial muscles, and wearable bioelectronic therapeutics.

Highly Stretchable Core-Sheath Fibers via Wet-Spinning for Wearable Strain Sensors.

Lightweight, stretchable, and wearable strain sensors have recently been widely studied for the development of health monitoring systems, human-machine interfaces, and wearable devices. Herein, highly stretchable polymer elastomer-wrapped carbon nanocomposite piezoresistive core-sheath fibers are successfully prepared using a facile and scalable one-step coaxial wet-spinning assembly approach. The carbon nanotube-polymeric composite core of the stretchable fiber is surrounded by an insulating sheath, similar to conventional cables, and shows excellent electrical conductivity with a low percolation threshold (0.74 vol %). The core-sheath elastic fibers are used as wearable strain sensors, exhibiting ultra-high stretchability (above 300%), excellent stability (>10 000 cycles), fast response, low hysteresis, and good washability. Furthermore, the piezoresistive core-sheath fiber possesses bending-insensitiveness and negligible torsion-sensitive properties, and the strain sensing performance of piezoresistive fibers maintains a high degree of stability under harsh conditions. On the basis of this high level of performance, the fiber-shaped strain sensor can accurately detect both subtle and large-scale human movements by embedding it in gloves and garments or by directly attaching it to the skin. The current results indicate that the proposed stretchable strain sensor has many potential applications in health monitoring, human-machine interfaces, soft robotics, and wearable electronics.

Ultrasensitive Wearable Soft Strain Sensors of Conductive, Self-healing, and Elastic Hydrogels with Synergistic "Soft and Hard" Hybrid Networks.

Robust, stretchable, and strain-sensitive hydrogels have recently attracted immense research interest because of their potential application in wearable strain sensors. The integration of the synergistic characteristics of decent mechanical properties, reliable self-healing capability, and high sensing sensitivity for fabricating conductive, elastic, self-healing, and strain-sensitive hydrogels is still a great challenge. Inspired by the mechanically excellent and self-healing biological soft tissues with hierarchical network structures, herein, functional network hydrogels are fabricated by the interconnection between a "soft" homogeneous polymer network and a "hard" dynamic ferric (Fe3+) cross-linked cellulose nanocrystals (CNCs-Fe3+) network. Under stress, the dynamic CNCs-Fe3+ coordination bonds act as sacrificial bonds to efficiently dissipate energy, while the homogeneous polymer network leads to a smooth stress-transfer, which enables the hydrogels to achieve unusual mechanical properties, such as excellent mechanical strength, robust toughness, and stretchability, as well as good self-recovery property. The hydrogels demonstrate autonomously self-healing capability in only 5 min without the need of any stimuli or healing agents, ascribing to the reorganization of CNCs and Fe3+ via ionic coordination. Furthermore, the resulted hydrogels display tunable electromechanical behavior with sensitive, stable, and repeatable variations in resistance upon mechanical deformations. Based on the tunable electromechanical behavior, the hydrogels can act as a wearable strain sensor to monitor finger joint motions, breathing, and even the slight blood pulse. This strategy of building synergistic "soft and hard" structures is successful to integrate the decent mechanical properties, reliable self-healing capability, and high sensing sensitivity together for assembling a high-performance, flexible, and wearable strain sensor.