Stretchable Conductive Materials Research Articles

Stretchable composites with electrical conductivity

Abstract Recently, the development of flexible and stretchable electronics has resulted in extensive studies focused on the investigation of elastic composites with various functions using stretchable materials, such as rubber. Among these materials, conductive composites using stretchable conductive materials can withstand larger deformations than solid metals and simultaneously retain their conductivity. Furthermore, such conductive composite materials can be imparted with various physical properties, such as thermal and magnetic properties (in addition to conductive properties), by changing the properties of the base and filler materials. Owing to these properties, conductive stretchable composites are expected to have various areas of applications, such as sensors, heaters, and magnetic barrier films, beyond electrical wiring on flexible and stretchable substrates with large deformations. This study reviewed flexible materials exhibiting both elasticity and conductivity with a particular focus on the internal filler material and functionality.

A Stretchable Conductive Material with High Fatigue Resistance for Strain Sensors.

Intrinsically stretchable conductive materials based on elastic substrates and conductive components play important roles in biomedical applications, such as exercise rehabilitation monitoring and disease prediction. A persistent challenge is to combine high fatigue resistance with excellent mechanical properties in stretchable conductive materials. Herein, we present a stretchable conductive material with both good fatigue resistance and high tensile properties (∼3170%) based on poly(acrylic acid)-phytic acid-trehalose-polypyrrole (denoted as PPTP). The as-prepared PPTP hydrogel electrode showed no obvious cracking or delamination after 400 loading and unloading cycles and maintained good electrical signal transmission function after 1000 cycles. We further collected stable signals for human motion and handwriting using the stretchable hydrogel electrode as a strain sensor, demonstrating the potential application of the PPTP stretchable hydrogel electrode in biomedicine.

Multifunctional ultraelastic helical conductive yarn for motion detection and human-machine interaction

Featured with intrinsic lightweight, great flexibility, and easy integration into functional textiles or devices, the stretchable conductive fiber has attracted much attention in the realm of wearable electronics. However, the conductive fibers encounter a troublesome “trade-off” between high conductivity and large elasticity under large deformation, which restricts their widespread applications. Herein, we designed a multifunctional highly elastic helical conductive yarn (HCY) by electrospinning polyurethane (PU) nanofibers, polydopamine (PDA)-assisted silver nanoparticles (AgNPs) deposition and over-twisting. The introduction of a PDA mediated layer fosters strong bond between the conductive AgNPs and the elastic PU nanofibers matrix, showcasing robust structural stability and electrical performance. The hierarchically interlocked conductive structure confers high electrical conductivity to the stretchable HCY, enabling it to withstand large mechanical deformation, which achieves good recoverability within a range of 700 %, great durability (40000 times at deformation of 200 %) and maximum conductive tensile elongation up to 1200 %. Furthermore, the HCY also features excellent Joule-heating ability, great antibacterial performance, and functions as a rapid-response strain sensor (GFmax = 9.82), which is ideal for detecting human motion and enhancing human–machine interactions. This work provides a new path for developing advanced stretchable conductive materials, which is of great significance for versatile ultraelastic wearable electronic devices.

Economically viable electromechanical tensile testing equipment for stretchable sensor assessment

The growing interest in soft robotics increases the demand for stretchable sensors. The high performance of stretchable sensors depends much on the linearity, reliability and hysteresis of the stretchable conductive materials. In the applications of conductive materials such as in dielectric elastomer actuators, a stretchable conductive material should maintain the conductivity while sustaining large and multiple cycles of stretch and release tests. To understand the stretchable electrode quality, researchers should perform an electromechanical test. However, researchers require a high investment cost to use a professional type of electromechanical tensile test. In this research, we proposed an economically viable version of the Do-it-yourself (DIY) electromechanical tensile test (EMTT) to resolve the high investment cost problems. The DIY-EMTT is based on the Arduino-nano module. We integrate the load cell, displacement sensor, motor linear stage and DIY resistance meter. We can use the DIY mechanism to suppress the instrumental cost from thousands to hundreds of dollars. Furthermore, we provide a step-by-step guide to build the DIY-EMTT. We expect our DIY-EMTT to boost stretchable sensor development in soft robotics.

Highly Biocompatible Antibacterial Hydrogel for Wearable Sensing of Macro and Microscale Human Body Motions.

Flexible electronics, like electronic skin (e-skin), rely on stretchable conductive materials that integrate diverse components to enhance mechanical, electrical, and interfacial properties. However, poor biocompatibility, bacterial infections, and limited compatibility of functional additives within polymer matrices hinder healthcare sensors' performance. This study addresses these challenges by developing an antibacterial hydrogel using polyvinyl alcohol (PVA), konjac glucomannan (KGM), borax (B), and flower-shaped silver nanoparticles (F-AgNPs), referred as PKB/F-AgNPs hydrogel. The developed hydrogel forms a hierarchical network structure, with a tensile strength of 96 kPa, 83% self-healing efficiency within 60 minutes, and 128% cell viability in Cell Counting Kit-8 (CCK-8) assays, indicating excellent biocompatibility. It also shows strong antibacterial efficacy against Gram-negative Escherichia coli (E. coli) and Gram-positive Staphylococcus aureus (S. aureus). Blue light irradiation enhances its antibacterial activity by 1.3-fold for E. coli and 2.2-fold for S. aureus. The hydrogel's antibacterial effectiveness is assessed by monitoring changes in electrical conductivity, providing a cost-effective alternative to traditional microbial culture assays. The PKB/F-AgNPs hydrogel's flexibility and electrical conductivity enable it to function as strain sensors for detecting body movements and facial expressions. This antibacterial hydrogel underscores its potential for future human-machine interfaces and wearable electronics.

Stretchable Sensor Materials Applicable to Radiofrequency Coil Design in Magnetic Resonance Imaging: A Review.

Wearable sensors are rapidly gaining influence in the diagnostics, monitoring, and treatment of disease, thereby improving patient outcomes. In this review, we aim to explore how these advances can be applied to magnetic resonance imaging (MRI). We begin by (i) introducing limitations in current flexible/stretchable RF coils and then move to the broader field of flexible sensor technology to identify translatable technologies. To this goal, we discuss (ii) emerging materials currently used for sensor substrates, (iii) stretchable conductive materials, (iv) pairing and matching of conductors with substrates, and (v) implementation of lumped elements such as capacitors. Applicable (vi) fabrication methods are presented, and the review concludes with a brief commentary on (vii) the implementation of the discussed sensor technologies in MRI coil applications. The main takeaway of our research is that a large body of work has led to exciting new sensor innovations allowing for stretchable wearables, but further exploration of materials and manufacturing techniques remains necessary, especially when applied to MRI diagnostics.

Recyclable and mechanically tough nanocellulose reinforced natural rubber composite conductive elastomers for flexible multifunctional sensor

The development of flexible wearable multifunctional electronics has gained great attention in the field of human motion monitoring. However, developing mechanically tough, highly stretchable, and recyclable composite conductive materials for application in multifunctional sensors remained great challenges. In this work, a mechanically tough, highly stretchable, and recyclable composite conductive elastomer with the dynamic physical-chemical dual-crosslinking network was fabricated by the combination of multiple hydrogen bonds and dynamic ester bonds. To prepare the proposed composite elastomers, the polyaniline-modified carboxylate cellulose nanocrystals (C-CNC@PANI) were used as both conductive filler to yield high conductivity of 15.08 mS/m, and mechanical reinforcement to construct the dynamic dual-crosslinking network with epoxidized natural rubber latex to realize the high mechanical strength (8.65 MPa) and toughness (29.57 MJ/m3). Meanwhile, the construction of dynamic dual-crosslinking network endowed the elastomer with satisfactory recyclability. Based on these features, the composite conductive elastomers were used as strain sensors, and electrode material for assembling flexible and recyclable self-powered sensors for monitoring human motions. Importantly, the composite conductive elastomers maintained reliable sensing and energy harvesting performance even after multiple recycling process. This study provides a new strategy for the preparation of recyclable, mechanically tough composite conductive materials for wearable sensors.

Bionic-leaf vein inspired breathable anti-impact wearable electronics with health monitoring, electromagnetic interference shielding and thermal management

Breathable and stretchable conductive materials are ideal for healthcare wearable electronic devices. However, the tradeoff between the sensitivity and detection range of electronic sensors and the challenge posed by simple-functional electronics limits their development. Here, inspired by the bionic-leaf vein conductive path, silver nanowires (AgNWs)-Ti3C2Tx (MXene) hybrid structure assembled on the nonwoven fabrics (NWF) is well sandwiched between porous polyborosiloxane elastomer (PBSE) to construct the multifunctional breathable wearable electronics with both high anti-impact performance and good sensing behavior. Benefiting from the high conductive AgNWs-MXene hybrid structure, the NWF/AgNWs-MXene/PBSE nanocomposite exhibits high sensitivity (GF = 1158.1), wide monitoring range (57 %), controllable thermal management properties, and excellent electromagnetic interference shielding effect (SET = 41.46 dB). Moreover, owing to the wonderful shear stiffening effect of PBSE, the NWF/AgNWs-MXene/PBSE possesses a high energy absorption performance. Combining with deep learning, this breathable electronic device can be further applied to wireless sensing gloves and multifunctional medical belts, which will drive the development of electronic skin, human-machine interaction, and personalized healthcare monitoring applications.

A highly sensitive and anti-freezing conductive strain sensor based on polypyrrole/cellulose nanofiber crosslinked polyvinyl alcohol hydrogel for human motion detection

Electro-conductive hydrogels emerge as a stretchable conductive materials with diverse applications in the synthesis of flexible strain sensors. However, the high-water content and low cross-links density cause them to be mechanically destroyed and freeze at subzero temperatures, limiting their practical applications. Herein, we report a one-pot strategy by co-incorporating cellulose nanofiber (CNF), Poly pyrrole (PPy) and glycerol with polyvinyl alcohol (PVA) to prepare hydrogel. The addition of PPy endowed the hydrogel with good conductivity (∼0.034 S/m) compared to the no PPy@CNF group (∼0.0095 S/m), the conductivity was increased by 257.9 %. The hydrogel exhibits comparable ionic conductivity at −18 °C as it does at room temperature. It's attributed to the glycerol as a cryoprotectant and the formation of hydrated [Zn(H2O)n]2+ ions via strong interaction between Zn2+ and water molecules. Moreover, the cellulose nanofiber intrinsically assembled into unique hierarchical structures allow for strong hydrogen bonds between adjacent cellulose and PPy polymer chains, greatly improve the mechanical strength (stress∼0.65 MPa, strain∼301 %) and excellent viscoelasticity (G'max ∼ 82.7 KPa). This novel PPy@CNF-PVA hydrogel exhibits extremely high Gauge factor (GF) of 2.84 and shows excellent sensitivity, repeatability and stability. Therefore, the hydrogel can serve as reliable and stable strain sensor which shows excellent responsiveness in human activities monitoration.

Tough soldering for stretchable electronics by small-molecule modulated interfacial assemblies

The rapid-developing soft robots and wearable devices require flexible conductive materials to maintain electric functions over a large range of deformations. Considerable efforts are made to develop stretchable conductive materials; little attention is paid to the frequent failures of integrated circuits caused by the interface mismatch of soft substrates and rigid silicon-based microelectronics. Here, we present a stretchable solder with good weldability that can strongly bond with electronic components, benefiting from the hierarchical assemblies of liquid metal particles, small-molecule modulators, and non-covalently crosslinked polymer matrix. Our self-solder shows high conductivity (>2×105 S m−1), extreme stretchability (~1000%, and >600% with chip-integrated), and high toughness (~20 MJ m−3). Additionally, the dynamic interactions within our solder’s surface and interior enable a range of unique features, including ease of integration, component substitution, and circuit recyclability. With all these features, we demonstrated an application as thermoforming technology for three-dimensional (3D) conformable electronics, showing potential in reducing the complexity of microchip interfacing, as well as scalable fabrication of chip-integrated stretchable circuits and 3D electronics.

Spider-Silk-Inspired Tough, Self-Healing, and Melt-Spinnable Ionogels.

As stretchable conductive materials, ionogels have gained increasing attention. However, it still remains crucial to integrate multiple functions including mechanically robust, room temperature self-healing capacity, facile processing, and recyclability into an ionogel-based device with high potential for applications such as soft robots, electronic skins, and wearable electronics. Herein, inspired by the structure of spider silk, a multilevel hydrogen bonding strategy to effectively produce multi-functional ionogels is proposed with a combination of the desirable properties. The ionogels are synthesized based on N-isopropylacrylamide (NIPAM), N, N-dimethylacrylamide (DMA), and ionic liquids (ILs) 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]). The synergistic hydrogen bonding interactions between PNIPAM chains, PDMA chains, and ILs endow the ionogels with improved mechanical strength along with fast self-healing ability at ambient conditions. Furthermore, the synthesized ionogels show great capability for the continuous fabrication of the ionogel-based fibers using the melt-spinning process. The ionogel fibers exhibit spider-silk-like features with hysteresis behavior, indicating their excellent energy dissipation performance. Moreover, an interwoven network of ionogel fibers with strain and thermal sensing performance can accurately sense the location of objects. In addition, the ionogels show great recyclability and processability into different shapes using 3D printing. This work provides a new strategy to design superior ionogels for diverse applications.

Research Progress in Stretchable Circuits: Materials, Methods, and Applications

AbstractStretchable electronic devices, with their excellent properties such as stretchability and conformal contact with complex surfaces, are widely used in health monitoring and human‐computer interactions. For stable operation of these devices, stretchable circuits are crucial, enabling integration of sensors, data collection, and transmission while under strain. To achieve stretchable system integration, addressing key issues such as elastic substrates, sensor devices, rigid components, stretchable electrodes, and packaging layers is necessary. The stretchable electrodes, which connect various functional devices, are crucial for achieving stretchability and are the main focus of this review. Firstly, this work explores the enhancement of electrode design to maintain good electrical conductivity even under stretching conditions, through studying stretchable conductive materials and the structural design of conventional materials. This work then presents studies on substrate interfaces and the design of elastic substrates, such as rigid islands, to enhance the stability of stretchable circuits during use. Finally, the article discusses the applications of stretchable circuits, the challenges they face, and provides new research directions and ways to develop stretchable circuits.

Tough, stretchable dual-network liquid metal-based hydrogel toward high-performance intelligent on-off electromagnetic interference shielding, human motion detection and self-powered application

The stretchable conductive materials with adjustable electromagnetic interference (EMI) shielding performance and other multifunctional integrated applications are remarkably desirable and challenging in flexible electronics. However, the existing stretchable materials often suffer from the decay of EMI shielding performance during the stretching process, which limits their practical applications. Meanwhile, it remains a great challenge to construct materials with ordered porous frameworks as integrated shielding devices. Incorporating porous structure will generate abundant interior surfaces/interfaces, facilitating multiple reflections of incident electromagnetic waves (EMWs). Herein, we employ ultrasound method to modify liquid metal (LM) with carbon nanotubes (CNTs), and further utilize an UV in-situ polymerization method to fabricate CNT@LM/polyacrylamide/gelatin (LMCPG) dual network hydrogel elastomer. The LMCPG hydrogel elastomer possesses high strength and durability, and its tensile strength reaches 117 kPa at 1033% strain owing to the high strength of the rigid network and the beneficial deformation ability of the flexible network. Deformable CNT@LM droplets elongate randomly during stretching process, which facilitates establishing more conductive paths. The EMI shielding capacity of the stretched elastomer can be controlled, achieving an intelligent on-off behavior, which exhibits a 211% increase at 200% strain in EMI shielding effectiveness (SE) compared with the undeformed state. Moreover, the LMCPG elastomer shows a significant triboelectric performance, which can provide power supply for flexible electronic devices, achieving an uninterrupted monitoring of the human body motion by devices. Therefore, as a flexible electronic material, it can offer a facile solution to achieve intelligent multifunctional integrated EMI shielding materials.

A Low‐Hysteresis and Highly Stretchable Ionogel Enabled by Well Dispersed Slidable Cross‐Linker for Rapid Human‐Machine Interaction

AbstractIonic conductive soft materials for mimicking human skin are a promising topic since they can be thought of as a possible basis for biomimetic sensing. In pursuit of devices with a long working range and low signal delay, conductive materials with low hysteresis and good stretchability are highly demanded. To overcome the challenges of highly stretchable conductive materials with good resilience, herein a chemical design is proposed where polyrotaxanes act as topological cross‐linkers to enhance the stretchability by sliding‐induced reduced stress concentration while the compatible ionic liquid is introduced as a dispersant for low hysteresis. The obtained ionogels exhibit versatile properties more than low hysteresis (residual strain = 7%) and good stretchability (550%), and also anti‐fatigue, biocompatibility, and good adhesion. The low hysteresis is attributed to lower energy dissipation from the well‐dispersed polyrotaxanes by compatible ionic liquids. The mechanism provides a new insight in fabricating highly stretchable and low‐hysteresis slide‐ring materials. Furthermore, the conductivity of the ionogels and their responses to strains and temperatures are measured. Benefiting from the good conductivity and low hysteresis, the ionogel is applied to develop a wireless communication system to realize rapid human‐machine interactions.

Stretchable conductive hydrogel with super resistance-strain stability and ultrahigh durability enabled by specificity crosslinking strategy for high-performance flexible electronics

Stretchable ionic conductive hydrogels (SICHs) are regarded as one of the indispensable components for flexible electronics desirable to provide stable signal transmission and functional reproducibility. However, the state-of-the-art SICHs demonstrate a narrow resistance-stability range and poor cyclical fatigue reliability due to ion migration limitations and the absence of the molecular design regime. Herein, we present a novel synthetic strategy that utilizes the dynamic Zn-carboxyl physical bonding, adjacent to B-hydroxyl chemical bonding, to realize the “specificity” cross-linking in pectin polymeric networks. This approach significantly extends the resistance-stability range of SICHs, while also providing remarkable longevity. Via “specificity” crosslinking design, the Zn-carboxyl physical bonding, bearing thermodynamically stable and dynamic exchange character, can break the resistance-strain dependence of ionic conductive hydrogel, offering an unprecedented resistance-stability under largely applied strain (300%). Moreover, the B-hydroxyl chemical bonding effectively overcomes the conductivity and mechanical strength trade-off dilemma due to its strong but dynamic feature, realizing the high durability of SICHs. In addition, the extraordinary tolerate harsh environment capacity was achieved by introducing glycerin to form rich hydrogen bonds in the SICHs network, which is crucial for the avoidance of congelation at subzero temperatures and dehydration resulting from the circuit heat. As a stretchable conductive component of deformable electronic devices, the SICH demonstrates extraordinary long life and stable operation. These observations reveal fresh stretchable conductive materials.

Silver-Nanowire-Based Elastic Conductors: Preparation Processes and Substrate Adhesion.

The production of flexible electronic systems includes stretchable electrical interconnections and flexible electronic components, promoting the research and development of flexible conductors and stretchable conductive materials with large bending deformation or torsion resistance. Silver nanowires have the advantages of high conductivity, good transparency and flexibility in the development of flexible electronic products. In order to further prepare system-level flexible systems (such as autonomous full-software robots, etc.), it is necessary to focus on the conductivity of the system's composite conductor and the robustness of the system at the physical level. In terms of conductor preparation processes and substrate adhesion strategies, the more commonly used solutions are selected. Four kinds of elastic preparation processes (pretensioned/geometrically topological matrix, conductive fiber, aerogel composite, mixed percolation dopant) and five kinds of processes (coating, embedding, changing surface energy, chemical bond and force, adjusting tension and diffusion) to enhance the adhesion of composite conductors using silver nanowires as current-carrying channel substrates were reviewed. It is recommended to use the preparation process of mixed percolation doping and the adhesion mode of embedding/chemical bonding under non-special conditions. Developments in 3D printing and soft robots are also discussed.

Characterization of Conductive Carbon Nanotubes/Polymer Composites for Stretchable Sensors and Transducers.

The increasing interest in stretchable conductive composite materials, that can be versatile and suitable for wide-ranging application, has sparked a growing demand for studies of scalable fabrication techniques and specifically tailored geometries. Thanks to the combination of the conductivity and robustness of carbon nanotube (CNT) materials with the viscoelastic properties of polymer films, in particular their stretchability, "surface composites" made of a CNT on polymeric films are a promising way to obtain a low-cost, conductive, elastic, moldable, and patternable material. The use of polymers selected for specific applications, however, requires targeted studies to deeply understand the interface interactions between a CNT and the surface of such polymer films, and in particular the stability and durability of a CNT grafting onto the polymer itself. Here, we present an investigation of the interface properties for a selected group of polymer film substrates with different viscoelastic properties by means of a series of different and complementary experimental techniques. Specifically, we studied the interaction of a single-wall carbon nanotube (SWCNT) deposited on two couples of different polymeric substrates, each one chosen as representative of thermoplastic polymers (i.e., low-density polyethylene (LDPE) and polypropylene (PP)) and thermosetting elastomers (i.e., polyisoprene (PI) and polydimethylsiloxane (PDMS)), respectively. Our results demonstrate that the characteristics of the interface significantly differ for the two classes of polymers with a deeper penetration (up to about 100 μm) into the polymer bulk for the thermosetting substrates. Consequently, the resistance per unit length varies in different ranges, from 1-10 kΩ/cm for typical thermoplastic composite devices (30 μm thick and 2 mm wide) to 0.5-3 MΩ/cm for typical thermosetting elastomer devices (150 μm thick and 2 mm wide). For these reasons, the composites show the different mechanical and electrical responses, therefore suggesting different areas of application of the devices based on such materials.

Highly stretchable and sensitive silicone composites with positive piezoconductivity using nickel powder and ionic liquid.

Conductive rubber composites are mixtures of stretchable rubber and conductive materials. They can achieve conductivity and high elasticity and are used in soft robots and wearable devices. In general, these composites exhibit high electrical resistance owing to their bonds between the fillers breaking during elongation. However, there are several types of composite materials that decrease resistance by increasing contact between the conductive materials during elongation through optimization of the shape and size of the filler. These composite materials can rapidly decrease the resistance and are expected to be applicable to switch in electric circuits and sensors. However, to use such composite materials in circuits, the electrical resistance at the time of resistance reduction must be sufficiently low to not affect the electric circuit. To achieve this, a considerable amount of filler must be mixed; however, this reduces the elasticity of the composite. Simultaneously achieving elasticity of the composite and a sufficient decrease in the resistance is challenging. This study developed a conductive rubber composite gel by mixing silicone rubber, ionic liquid, and metal filler. Consequently, the composite achieved an elongation rate of over six times and a decrease in the resistance of less than 1/105. In addition, this composite material was used as a switch circuit wherein an electric circuit is turned on and off according to elongation through a connection to a DC power source.

Internally Structured Conductive Composite for Reliable Stretchable Electronics (Adv. Electron. Mater. 2/2023)

Reliable Stretchable Conductor The process using a hydrophilic liquid improves the reliability of stretchable conductive composite materials. This process forms an internal structure that consumes strain during stretching, thereby minimizing the changes in resistance during cyclic stretching and maximizing elastic durability. It also improves conductivity by concentrating conductive fillers to increase the number of conductive paths. More details can be found in article number 2201021 by Sungmook Jung and co-workers.

Multimaterial Three-Dimensional Printing of Ultraviolet-Curable Ionic Conductive Elastomers with Diverse Polymers for Multifunctional Flexible Electronics.

Ionic conductive elastomers (ICEs) are emerging stretchable and ionic conductive materials that are solvent-free and thus demonstrate excellent thermal stability. Three-dimensional (3D) printing that creates complex 3D structures in free forms is considered as an ideal approach to manufacture sophisticated ICE-based devices. However, the current technologies constrain 3D printed ICE structures in a single material, which greatly limits functionality and performance of ICE-based devices and machines. Here, we report a digital light processing (DLP)-based multimaterial 3D printing capability to seemly integrate ultraviolet-curable ICE (UV-ICE) with nonconductive materials to create ionic flexible electronic devices in 3D forms with enhanced performance. This unique capability allows us to readily manufacture various 3D flexible electronic devices. To demonstrate this, we printed UV-ICE circuits into polymer substrates with different mechanical properties to create resistive strain and force sensors; we printed flexible capacitive sensors with high sensitivity (2 kPa-1) and a wide range of measured pressures (from 5 Pa to 550 kPa) by creating a complex microstructure in the dielectric layer; we even realized ionic conductor-activated four-dimensional (4D) printing by printing a UV-ICE circuit into a shape memory polymer substrate. The proposed approach paves a new efficient way to realize multifunctional flexible devices and machines by bonding ICEs with other polymers in 3D forms.