Transparent,Highly Stretchable,Rehealable, Sensing,and Fully Recyclable Ionic Conductors Fabricated by One‐Step Polymerization Based on a Small Biological Molecule

To date, various stretchable conductors have been fabricated, but simultaneous realization of the transparency, high stretchability, electrical conductivity, self‐healing capability, and sensing property through a simple, fast, cost‐efficient approach is still challenging. Here, α‐lipoic acid (LA), a naturally small biological molecule found in humans and animals, is used to fabricate transparent (>85%), electrical conductivity, highly stretchable (strain up to 1100%), and rehealable (mechanical healing efficiency of 86%, electrical healing efficiency of 96%) ionic conductor by solvent‐free one‐step polymerization. Furthermore, the ionic conductors with appealing sensitivity can be served as strain sensors to detect and distinguish various human activities. Notably, this ionic conductor can be fully recycled and reprocessed into new ionic conductors or adhesives by a direct heating process, which offers a promising prospect in great reduction of electronic wastes that have brought acute environmental pollution. In consideration of the extremely facile preparation process, biological available materials, satisfactory functionalities, and full recyclability, the emergence of LA‐based ionic conductors is believed to open up a new avenue for developing sustainable and wearable electronic devices in the future.     

Stretchable Interconnects for Elastic Electronic Surfaces

Elastic electronic surfaces will integrate stiff thin film devices onto compliant polymer substrates. These surfaces may be stretched once or many times, by up to tens of percent strain. One way to make such an elastic electronic surface is to distribute rigid subcircuit islands over the polymer surface, and then fabricate active devices on the islands. These islands need to be interconnected with stretchable metallization. We describe stretchable interconnects made of stripes of thin gold film patterned on elastomeric membranes. These membranes can be stretched by up to twice their initial length and maintain electrical conduction. We review the fabrication of these conductors, present their electrical and mechanical properties, and summarize our model for their extreme stretchability. Using such stretchable interconnects, we made the first elastic circuit, an inverter of thin film transistors. The circuit remains functional when stretched and relaxed by 12% strain.     

Self‐Healing and Stretchable 3D‐Printed Organic Thermoelectrics

With the advent of flexible and wearable electronics and sensors, there is an urgent need to develop energy‐harvesting solutions that are compatible with such wearables. However, many of the proposed energy‐harvesting solutions lack the necessary mechanical properties, which make them susceptible to damage by repetitive and continuous mechanical stresses, leading to serious degradation in device performance. Developing new energy materials that possess high deformability and self‐healability is essential to realize self‐powered devices. Herein, a thermoelectric ternary composite is demonstrated that possesses both self‐healing and stretchable properties produced via 3D‐printing method. The ternary composite films provide stable thermoelectric performance during viscoelastic deformation, up to 35% tensile strain. Importantly, after being completely severed by cutting, the composite films autonomously recover their thermoelectric properties with a rapid response time of around one second. Using this self‐healable and solution‐processable composite, 3D‐printed thermoelectric generators are fabricated, which retain above 85% of their initial power output, even after repetitive cutting and self‐healing. This approach represents a significant step in achieving damage‐free and truly wearable 3D‐printed organic thermoelectrics.     

Highly Sensitive,Wearable, Durable Strain Sensors and Stretchable Conductors Using Graphene/Silicon Rubber Composites

Highly sensitive, wearable and durable strain sensors are vital to the development of health monitoring systems, smart robots and human machine interfaces. The recent sensor fabrication progress is respectable, but it is limited by complexity, low sensitivity and unideal service life. Herein a facile, cost‐effective and scalable method is presented for the development of high‐performance strain sensors and stretchable conductors based on a composite film consisting of graphene platelets (GnPs) and silicon rubber. Through calculation by the tunneling theory using experimental data, the composite film has demonstrated ideal linear and reproducible sensitivity to tensile strains, which is contributed by the superior piezoresistivity of GnPs having tunable gauge factors 27.7–164.5. The composite sensors fabricated in different days demonstrate pretty similar performance, enabling applications as a health‐monitoring device to detect various human motions from finger bending to pulse. They can be used as electronic skin, a vibration sensor and a human‐machine interface controller. Stretchable conductors are made by coating and encapsulating GnPs with polydimethyl siloxane to create another composite; this structure allows the conductor to be readily bent and stretched with sufficient mechanical robustness and cyclability.     

An Intrinsically Stretchable High‐Performance Polymer Semiconductor with Low Crystallinity

For wearable and implantable electronics applications, developing intrinsically stretchable polymer semiconductor is advantageous, especially in the manufacturing of large‐area and high‐density devices. A major challenge is to simultaneously achieve good electrical and mechanical properties for these semiconductor devices. While crystalline domains are generally needed to achieve high mobility, amorphous domains are necessary to impart stretchability. Recent progresses in the design of high‐performance donor–acceptor polymers that exhibit low degrees of energetic disorder, while having a high fraction of amorphous domains, appear promising for polymer semiconductors. Here, a low crystalline, i.e., near‐amorphous, indacenodithiophene‐co‐benzothiadiazole (IDTBT) polymer and a semicrystalline thieno[3,2‐b]thiophene‐diketopyrrolopyrrole (DPPTT) are compared, for mechanical properties and electrical performance under strain. It is observed that IDTBT is able to achieve both a high modulus and high fracture strain, and to preserve electrical functionality under high strain. Next, fully stretchable transistors are fabricated using the IDTBT polymer and observed mobility ≈0.6 cm² V^?1 s^?1 at 100% strain along stretching direction. In addition, the morphological evolution of the stretched IDTBT films is investigated by polarized UV–vis and grazing‐incidence X‐ray diffraction to elucidate the molecular origins of high ductility. In summary, the near‐amorphous IDTBT polymer signifies a promising direction regarding molecular design principles toward intrinsically stretchable high‐performance polymer semiconductor.     

3D Interconnected Conductive Graphite Nanoplatelet Welded Carbon Nanotube Networks for Stretchable Conductors

Stretchable conductors with stable electrical conductivity under harsh mechanical deformations are essential for developing next generation portable and flexible wearable electronics. To achieve both high stretchability and conductivity with electromechanical stability, highly stretchable conductors based on 3D interconnected conductive graphite nanoplatelet welded carbon nanotube (GNP-w-CNT) networks are fabricated by welding the junctions of CNTs using GNPs followed by infiltrating with poly(dimethylsiloxane) (PDMS). It is observed that GNPs can weld the adjacent CNTs to facilitate the formation of continuous conductive pathways and avoid interfacial slippage under repetitive stretching. The enhanced interfacial bonding enables the conductor both high electrical conductivity (>132 S m⁻¹) and high stretchability (>150% strain) while ensuring long-term stability (1000 stretching-releasing cycles under 60% tensile strain). To demonstrate the outstanding flexibility and electrical stability, a flexible and stretchable light-emitting diode circuit with stable performance during stretching, bending, twisting, and pressing conditions is further fabricated. The unique welding mechanism can be easily extended to other material systems to broaden the application of stretchable conductors to a myriad of new applications.     

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.     

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.     

Highly Stretchable or Transparent Conductor Fabrication by a Hierarchical Multiscale Hybrid Nanocomposite

As is frequently seen in sci‐fi movies, future electronics are expected to ultimately be in the form of wearable electronics. To realize wearable electronics, the electric components should be soft, flexible, and even stretchable to be human‐friendly. An important step is presented toward realization of wearable electronics by developing a hierarchical multiscale hybrid nanocomposite for highly flexible, stretchable, or transparent conductors. The hybrid nanocomposite combines the enhanced mechanical compliance, electrical conductivity, and optical transparency of small CNTs (d ≈ 1.2 nm) and the enhanced electrical conductivity of relatively bigger Ag nanowire (d ≈ 150 nm) backbone to provide efficient multiscale electron transport path with Ag nanowire current backbone collector and local CNT percolation network. The highly elastic hybrid nanocomposite conductors and highly transparent flexible conductors can be mounted on any non‐planar or soft surfaces to realize human‐friendly electronics interface for future wearable electronics.     

Design and performance of thin metal film interconnects for skin-like electronic circuits

We prepare stretchable electrical conductors of 25-nm-thick gold films on elastomeric substrates prestretched by 15%. When the substrates relax from the prestretch, the gold stripes form surface waves with /spl sim/8.4-/spl mu/m wavelength and /spl sim/1.2-/spl mu/m amplitude. When the strain is cycled between 0 and 15%, both the wave pattern and the electrical resistance of the gold stripes change in reproducible cycles. Such repeatedly stretchable metallization can serve as interconnects for skin-like, conformal, and electroactive polymer circuits.     

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.     

Self‐Healable and Stretchable Organic Thermoelectric Materials: Electrically Percolated Polymer Nanowires Embedded in Thermoplastic Elastomer Matrix

Self‐healable and stretchable energy‐harvesting materials can provide a new avenue for the realization of self‐powered wearable electronics, including electronic skins, whose main materials are required to be robust to and stable under external damage and severe mechanical stresses. However, thermoelectric (TE) materials showing both self‐healing properties and stretchability have not yet been demonstrated despite their great potential to harvest thermal energy in the human body. As most existing TE materials are either mechanically brittle or unrecoverable after being subjected to damage, a novel approach is necessary for designing such materials. Herein, self‐healable and stretchable TE materials based on all‐organic composite system wherein polymer semiconductor nanowires are p‐doped with a molecular dopant and embedded in a thermoplastic elastomer matrix are reported. The polymer nanowires are electrically percolated in the matrix, and the resulting composite materials exhibit good TE performance. The composites also exhibit both excellent self‐healing properties under mild heat and pressure conditions and good stretchability. It is believed that this work can be a cornerstone for the design of self‐healable and stretchable energy‐harvesting materials as it provides useful guidelines for imparting electrical conductivity to insulating thermoplastic elastomers, which typically possess versatile and useful mechanical properties.     

Anisotropic Thermal Conductive Composite by the Guided Assembly of Boron Nitride Nanosheets for Flexible and Stretchable Electronics

Owing to the growing demand for highly integrated electronics, anisotropic heat dissipation of thermal management material is a challenging and promising technique. Moreover, to satisfy the needs for advancing flexible and stretchable electronic devices, maintaining high thermal conductivity during the deformation of electronic materials is at issue. Presented here is an effective assembly technique to realize a continuous array of boron nitride (BN) nanosheets on tetrahedral structures, creating 3D thermal paths for anisotropic dissipation integrated with deformable electronics. The tetrahedral structures, with a fancy wavy shaped cross‐section, guarantee flexibility and stretchability, without the degradation of thermal conductivity during the deformation of the composite film. The structured BN layer in the composites induces a high thermal conductivity of 1.15 W m^?1 K^?1 in the through‐plane and 11.05 W m^?1 K^?1 in the in‐plane direction at the low BN fraction of 16 wt%, which represent 145% and 83% increases over the randomly mixing method, respectively. Furthermore, this structured BN composite maintains thermal dissipation property with 50% strain of the original length of composite. Various electronic device demonstrations provide exceptional heat dissipation capabilities, including thin film silicon transistor and light‐emitting diode on flexible and stretchable composite, respectively.     

Buckled Conductive Polymer Ribbons in Elastomer Channels as Stretchable Fiber Conductor

Conductors that can sustain large strains without change in resistance are highly needed for wearable electronic systems. Here, the fabrication of highly stretchable coaxial fiber conductors through self‐buckling of conductive polymer ribbons inside thermoplastic elastomer channels, using a “solution stretching–drying–buckling” process, is reported. The unique hierarchically buckled and conductive core in the axial direction makes the resistance of the fiber very stable, with less than 4% change when applying as much as 680% strain. These fibers can then be directly used as stretchable electrical interconnects or wearable heaters.     

Liquid Metal Based Island‐Bridge Architectures for All Printed Stretchable Electrochemical Devices

The adoption of epidermal electronics into everyday life requires new design and fabrication paradigms, transitioning away from traditional rigid, bulky electronics towards soft devices that adapt with high intimacy to the human body. Here, a new strategy is reported for fabricating achieving highly stretchable “island‐bridge” (IB) electrochemical devices based on thick‐film printing process involving merging the deterministic IB architecture with stress‐enduring composite silver (Ag) inks based on eutectic gallium‐indium particles (EGaInPs) as dynamic electrical anchors within the inside the percolated network. The fabrication of free‐standing soft Ag‐EGaInPs‐based serpentine “bridges” enables the printed microstructures to maintain mechanical and electrical properties under an extreme (≈800%) strain. Coupling these highly stretchable “bridges” with rigid multifunctional “island” electrodes allows the realization of electrochemical devices that can sustain high mechanical deformation while displaying an extremely attractive and stable electrochemical performance. The advantages and practical utility of the new printed Ag‐liquid metal‐based island‐bridge designs are discussed and illustrated using a wearable biofuel cell. Such new scalable and tunable fabrication strategy will allow to incorporate a wide range of materials into a single device towards a wide range of applications in wearable electronics.     

Stretchable,Transparent, and Thermally Stable Triboelectric Nanogenerators Based on Solvent‐Free Ion‐Conducting Elastomer Electrodes

The development of stretchable/soft electronics requires power sources that can match their stretchability. In this study, a highly stretchable, transparent, and environmentally stable triboelectric nanogenerator with ionic conductor electrodes (iTENG) is reported. The ion‐conducting elastomer (ICE) electrode, together with a dielectric elastomer electrification layer, allows the ICE‐iTENG to achieve a stretchability of 1036% and transmittance of 91.5%. Most importantly, the ICE is liquid solvent‐free and thermally stable up to 335 °C, avoiding the dehydration‐induced performance degradation of commonly used hydrogels. The ICE‐iTENG shows no decrease in electrical output even after storing at 100 °C for 15 h. Biomechanical motion energies are demonstrated to be harvested by the ICE‐iTENG for powering wearable electronics intermittently without extra power sources. An ICE‐iTENG‐based pressure sensor is also developed with sensitivity up to 2.87 kPa^?1. The stretchable ICE‐iTENG overcomes the strain‐induced performance degradation using percolated electrical conductors and liquid evaporation‐induced degradation using ion‐conducting hydrogels/ionogels, suggesting great promising applications in soft/stretchable electronics under a relatively wider temperature range.     

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.     

Liquid Metal based Stretchable Room Temperature Soldering Sticker Patch for Stretchable Electronics Integration (Adv. Funct. Mater. 36/2023)

Researchers are eagerly developing various stretchable conductors to fabricate devices for next-generation electronics. Most of the major problems in stretchable electronics happen at the connection between rigid and soft parts and the development of reliable soldering material is a major hurdle in stretchable electronics. Though there are attempts to devise new soldering processes for integrating chips and stretchable conductors, they still possess limitations such as mechanical stability, mass production, sophisticated processes, and restricted candidates for conductors and substrates. Here, this study presents a room-temperature universal stretchable sticker-like soldering process that can stretchably solder multiple spots at once and directly fabricates a stretchable device in an in situ manner while a target conductor is installed on one's body. The solder developed in this research possesses high conductivity with a unique freestanding feature enabling the process. It can be elongated when directly positioned between a rigid chip and a rigid conductor, demonstrating its extraordinary stretchability. It is expected that this simple but unique stretchable soldering technique utilizing the invented solder will allow the integration of functional stretchable conductors with highly advanced rigid chips for next-generation stretchable electronics.     

Toward Macroscale,Isotropic Carbons with Graphene‐Sheet‐Like Electrical and Mechanical Properties

Realization of macroscale three‐dimensional isotropic carbons that retain the exceptional electrical and mechanical properties of graphene sheets remains a challenge. Here, a method for fabricating graphene‐derived carbons (GDCs) with isotropic properties approaching those of individual graphene sheets is reported. This synthesis scheme relies on direct cross‐linking of graphene sheets via the functional groups in graphene oxide to maximize electronic transport and mechanical reinforcement between sheets and the partial restacking of the sheets to increase the material density to about 1 g cm^‐3. These GDCs exhibit properties 3–6 orders of magnitude higher than previously reported 3D graphene assemblies.