Injectable and moldable hydrogels for use in sensitive and wide range strain sensing applications.

Recently, the use of hybrid double network (DN) hydrogels has become prominent due to their enhanced mechanical properties, which has opened the door for new applications of these soft materials. Only a few of these gels have demonstrated both injectable and moldable capabilities. In this work, we report the mechanical properties, gauge factor (GF) values and demonstrate both the injectability and moldability of a gelatin/polyacrylamide DN hydrogel. We optimized several parameters, such as, gelatin to polyacrylamide ratio, reactant concentrations and metal ion concentration, to produce a gelatin/polyacrylamide hydrogel with superior mechanical properties. The highest water content gel was capable of withstanding strains of 5000% before failure. These gels were facilely injected into molds where they effectively changed shape and maintained similar properties prior to remolding. When 20 mM calcium was doped into a similar gel, a tensile strength of 1.71 MPa was achieved. Aside from improving the mechanical properties of the gels, both Ca2+ and Mg2+ also improved their conductivity, so they were tested for use as strain sensors. The sensitivity of the hydrogel strain sensors were measured using the GF. For the 20 mM Ca2+ hydrogel, these GF values ranged from 1.63 to 6.85 for strains of 100% to 2100% respectively. Additionally, the sensors showed good stability over continuous cyclic stretching, demonstrating their long term reliability for strain sensing.

Highly Stretchable Capacitive Sensor with Printed Carbon Black Electrodes on Barium Titanate Elastomer Composite.

Wearable electronics and soft robotics are emerging fields utilizing soft and stretchable sensors for a variety of wearable applications. In this paper, the fabrication of a highly stretchable capacitive sensor with a printed carbon black/Ecoflex interdigital capacitor is presented. The highly stretchable capacitive sensor was fabricated on a substrate made from barium titanate⁻EcoflexTM 00-30 composite, and could withstand stretching up to 100%. The designed highly stretchable capacitive sensor was robust, and showed good repeatability and consistency when stretched and relaxed for over 1000 cycles.

Seconds Timescale Synthesis of Highly Stretchable Antibacterial Hydrogel for Skin Wound Closure and Epidermal Strain Sensor.

Effective wound healing is critical for patient care, and the development of novel wound dressing materials that promote healing, prevent infection, and are user-friendly is of great importance, particularly in the context of point-of-care testing (POCT). This study reports the synthesis of a hydrogel material that can be produced in less than 10 s and possesses antibacterial activity against both gram-negative and gram-positive microorganisms, as well as the ability to inhibit the growth of eukaryotic cells, such as yeast. The hydrogel is formed wholly based on covalent-like hydrogen bonding interactions and exhibits excellent mechanical properties, with the ability to stretch up to more than 600% of its initial length. Furthermore, the hydrogel demonstrates ultra-fast self-healing properties, with fractures capable of being repaired within 10 s. This hydrogel can promote skin wound healing, with the added advantage of functioning as a strain sensor that generates an electrical signal in response to physical deformation. The strain sensor composed of a rubber shell realizes fast and responsive strain sensing. The findings suggest that this hydrogel has promising applications in the field of POCT for wound care, providing a new avenue for improved patient outcomes.

A highly stretchable smart dressing for wound infection monitoring and treatment.

Smart dressings integrated with bioelectronics have attracted considerable attention and become promising solutions for skin wound management. However, due to the mechanical distinction between human body and the interface of electronics, previous smart dressings often suffered obvious degradation in electrical performance when attached to the soft and curvilinear wound sites. Here, we report a stretchable dressing integrated with temperature and pH sensor for wound status monitoring, as well as an electrically controlled drug delivery system for infection treatment. The wound dressing was featured with the deployment of liquid metal for seamless connection between rigid electrical components and gold particle-based electrodes, achieving a stretchable soft-hard interface. Stretching tests showed that both the sensing system and drug delivery system exhibited good stretchability and long-term stable conductivity with the resistance change rate less than 6 % under 50 % strain. Animal experiments demonstrated that the smart dressing was capable of detecting bacterial infection via the biomarkers of temperature and pH value and the infection factors of wound were significantly improved with therapy through electrically controlled antibiotics releasing. This proof-of-concept prototype has potential to significantly improve management of the wound, especially those with dynamic strain.

Highly Stretchable, Swelling-Resistant, Self-Healed, and Biocompatible Dual-Reinforced Double Polymer Network Hydrogels.

Superior flexibility and toughness can be achieved in bioactive hydrogels by the use of a double polymer network with complementary properties. Inspired by this design principle, we here combine polyacrylic acid (PAA) and sodium alginate (SA) to obtain a dual-reinforced double interpenetrating network (d-DIPN) hydrogel. The dual reinforcement involves ionic cross-linking and introduction of SiO2 nanoparticles, which leads to extraordinary improvements in strength and toughness. Compared with the standard PAA hydrogel that offers an elongation of 240% and a breakage stress of 0.03 MPa, the prepared SA(Ca2+)-PAA-SiO2 hydrogel shows an elongation above 1000% and a breakage stress of 1.62 MPa. Moreover, the combination of strong covalent cross-links and weak reversible interactions provides the d-DIPN hydrogel with swelling resistance and self-healing behavior, adhesive abilities, and shape memory performance. Furthermore, we show that the biocompatibility and bone cell proliferation ability of the hydrogels can be improved through a mineralization process despite an observed reduction in breakage strain and stress. Taken as a whole, our work paves the way for the design of strong and tough hydrogels, with potential applications within biomedicine and particularly tissue engineering.

Mechanically Tough and Highly Stretchable Hydrogels Based on Polyurethane for Sensitive Strain Sensor.

Hydrogels with flexible and stretchable properties are ideal for applications in wearable sensors. However, traditional hydrogel-based sensors suffer from high brittleness and low electrical sensitivity. In this case, to solve this dilemma, a macromolecular polyurethane crosslinking agent (PCA) was designed and prepared; after that, PCA and two-dimensional (2D) MXene nanosheets were both introduced into a covalently crosslinked network to enhance the comprehensive mechanical and electrochemical properties of the hydrogels. The macromolecular polyurethane crosslinking agent promotes high-tensile strength and highly stretchable capacity by suitable covalent crosslinking. The optimized hydrogel, which exhibited maximum tensile strength and maximum elongation at break, had results of 1.21 MPa and 644%, respectively. Two-dimensional MXene nanosheets provide hydrogel with high electrical conductivity and strain sensitivity, producing a wearable device for the continuous monitoring of human movements and facial microexpressions. This study demonstrated an efficient structure design strategy for building mechanically tough, highly stretchable, and sensitive dual-mode MXenes-based wearable sensors.

All Knitted and Integrated Soft Wearable of High Stretchability and Sensitivity for Continuous Monitoring of Human Joint Motion.

E-textiles have recently gained significant traction in the development of soft wearables for healthcare applications. However, there have been limited works on wearable e-textiles with embedded stretchable circuits. Here, stretchable conductive knits with tuneable macroscopic electrical and mechanical properties are developed by varying the yarn combination and the arrangement of stitch types at the meso-scale. Highly extensible piezoresistive strain sensors are designed (>120% strain) with high sensitivity (gauge factor 8.47) and durability (>100,000 cycles), interconnects (>140% strain) and resistors (>250% strain), optimally arranged to form a highly stretchable sensing circuit. The wearable is knitted with a computer numerical control (CNC) knitting machine that offers a cost effective and scalable fabrication method with minimal post-processing. The real-time data from the wearable is transmitted wirelessly using a custom designed circuit board. In this work, an all knitted and fully integrated soft wearable is demonstrated for wireless and continuous real-time sensing of knee joint motion of multiple subjects performing various activities of daily living.

Wearable and Stretchable SEBS/CB Polymer Conductive Strand as a Piezoresistive Strain Sensor.

A wearable and stretchable strain sensor with a gauge factor above 23 was prepared using a simple and effective technique. Conducting nanocomposite strands were prepared from styrene-b-(ethylene-co-butylene)-b-styrene triblock copolymer (SEBS) and carbon black (CB) through a solvent-processing method that uses a syringe pump. This novel nanocomposite preparation technique is a straightforward and cost-effective process and is reported in the literature for the first time. The work included two stages: the flexible nanocomposite preparation stage and the piezoresistive sensor stage. Depending on its molecular structure, the thermoelastic polymer SEBS is highly resilient to stress and strain. The main aim of this work is to fabricate a highly flexible and piezoresistive nanocomposite fibre/strand. Among the prepared composites, a composite corresponding to a composition just above the percolation threshold was selected to prepare the strain sensor, which exhibited good flexibility and conductivity and a large piezoresistive effect that was linearly dependent on the applied strain. The prepared nanocomposite sensor was stitched onto a sports T-shirt. Commercially available knee and elbow sleeves were also purchased, and the nanocomposite SEBS/CB strands were sewn separately on the two sleeves. The results showed a high sensitivity of the sensing element in the case of breathing activity (normal breathing, a 35% change, and deep breathing at 135%, respectively). In the case of knee and elbow movements, simultaneous measurements were performed and found that the sensor was able to detect movement cycles during walking.

High-performance carboxymethyl cellulose-based hydrogel film for food packaging and preservation system.

Most traditional food packaging and preservation films suffer from limited stretchability and relatively simple functionality, which severely restricts their practical application. In this study, a highly stretchable and versatile sodium carboxymethyl cellulose (CMC)/polyvinyl alcohol (PVA)/poly(ethylene imine) (PEI)/tannic acid (TA) hydrogel film was elaborately designed and demonstrated as an efficient food packaging and preservation system. The dynamic reversible non-covalent within three-dimensional (3D) network structures served as sacrificial bonds to dissipate the loaded energy and endowed the hydrogel film with excellent elongation ~400 %, which is much larger than that of conventional food packaging films (<50 %). Furthermore, the optimized CMC/PVA/PEI/TA3 hydrogel film delivers versatile performances, including self-healing, whole UV-blocking (<400 nm), strong adhesive strength (234.08 KPa), antioxidation virtues, oxygen barrier (32.64 cm3*µm/(m2*d*KPa)) and water vapor barrier (642.92 g/(m2*24 h)). Notably, the shelf life of fresh strawberries, mangoes, and cherries was prolonged by at least one week under ambient conditions when the packaging box was covered by the fabricated CMC/PVA/PEI/TA3 film. Thus, our work not only provides a highly stretchable and versatile hydrogel film but also boosts the in-depth comprehension and rational design of robust food packaging and preservation films.

Highly Stretchable Fully Biomass Autonomic Self-Healing Polyamide Elastomers and Their Foam for Selective Oil Absorption.

Renewable polymers with self-healing ability, excellent elongation, hydrophobicity, and selective oil absorption attributes are of interest for an extensive range of applications, such as e-skin, soft robots, wearable devices, and cleaning up oil spills. Herein, two fully renewable eco-friendly polyamide (PA)-based self-healing elastomers (namely, PA36,IA, and PA36,36) were prepared by a facile and green one-pot melt polycondensation of itaconic acid (IA), PripolTM 1009, and PriamineTM 1075 monomers. The molecular structures of these PAs were analyzed by FITR, 1H NMR, and 13C NMR. The distinct structure of these PAs shows superior strain values (above 2300%) and high ambient temperature autonomous self-healing ability. Interestingly, the synthesized renewable PA36,36 showed zero water absorption values and hydrophobic properties with a contact angle of θ = 91° compared to the synthesized PA36,IA and other previously reported PAs. These excellent attributes are due to the low concentration of amide groups, the highly entangled main chains, the intermolecular diffusion, the manifold dangling chains, and the numerous reversible physical bonds within the renewable PAs. Furthermore, the hydrophobic properties may aid in the selective oil absorption of the PA36,36-based foam, for which PA36,36 foam is produced by the green supercritical carbon dioxide (scCO2) batch foaming process. The PA36,36 foam with a microporous cellular structure showed better absorption capacity and high stability in repeated use. Due to these advantages, these bio-based PAs have potential for the production of eco-friendly self-healing materials, superabsorbent foams, and other polymeric materials.

A Highly Stretchable, Self-Healing Elastomer with Rate Sensing Capability Based on a Dynamic Dual Network.

Flexible sensing materials have attracted tremendous attention in recent years because of their potential applications in the fields of health monitoring, artificial intelligence, and so on. However, the preparation of rate sensing materials with self-healing performance is always a huge challenge. Herein, we first report the design and synthesis of a highly stretchable, recyclable, self-healing polysiloxane elastomer with rate sensing capability. The elastomer is composed of a dynamic dual network with boron/oxygen dative bonds and hydrogen bonds, which overcomes the structural instability of conventional solid-liquid materials. It exhibits certain adhesion, satisfactory mechanical robustness, and superior elongation at break (up to 1171%). After heating treatment at 80 °C for 2-4 h, the mechanical properties of damaged materials can be almost completely restored. Because of the "solid-liquid" property of the elastomer, it has irreplaceable functions which can sense different rates by resistance change after blending with multiwalled carbon nanotubes, principally in the range of 10 mm/min-150 mm/min. Especially, this rate sensing elastomer can be personalized by 3D printing at room temperature. This rate sensing strategy coupled with the introduction of dynamic dual-network structure is expected to help design advanced wearable devices for human rhythmic movement.

Highly stretchable and tough alginate-based cyclodextrin/Azo-polyacrylamide interpenetrating network hydrogel with self-healing properties.

Most structural self-healing materials were developed based on either reversible supramolecular interaction or dynamic covalent bonding. It seems a good idea to incorporate self-healing properties into high-performance materials. In this study, we fabricated the alginate-based cyclodextrin and polyacrylamide azobenzene highly stretchable and tough interpenetrating composite hydrogel with self-repairing behavior under light irradiation. Initially, the alginate-based cyclodextrin and polyacrylamide azobenzene were designed and synthesized. The corresponding structural, thermal, and morphological properties of hydrogels were characterized. The reversible transformation of the sol-gel can be achieved by the irradiation upon ultraviolet light and visible light. The self-healing behavior of this composited gel is based on the host-guest interaction between cyclodextrin and azobenzene. The recovery gel elongation at 48 h healing in the dark condition was is 0.04 MPa, with an elongation of 1140 %. Therefore, this gel can achieve self-healing ability while maintaining highly stretchable and tough performance.

Highly Stretchable and Fast Self-Healing Luminescent Materials.

Nowadays, the flourishing exploitation of multifunction luminescent materials with fast self-healing and superior mechanical features greatly broadens the scope for wide applications in optical and display devices, but this is still a formidably challenging task. Herein, we realize color-tunable luminescent materials functionalized with lanthanide ions (Ln3+) and terpyridine ligand coordination complexes that show highly stretchable and rapid self-healing performance, simultaneously broadening their application prospects both optically and mechanically. The multiple color emission, including visible and near-infrared luminescence, can be achieved by energy transfer from the coordinating terpyridine unit to Ln3+ via the so-called "antenna effect". The dynamic Ln-N coordination exhibits extreme stretchability and fast self-healing under ambient conditions. Of particular interest is that the healing process is not significantly affected by surface aging and atmospheric moisture. The multifunction materials open up a new pathway for future development of the next-generation wearable electronics including flexible and self-healable conductors.

Achieving High-Speed Retraction in Stretchable Hydrogels.

Hydrogels mimicking elastomeric biopolymers such as resilin, responsible for power-amplified activities in biological species necessary for locomotion, feeding, and defense have applications in soft robotics and prosthetics. Here, we report a bioinspired hydrogel synthesized through a free-radical polymerization reaction. By maintaining a balance between the hydrophilic and hydrophobic components, we obtain gels with an elastic modulus as high as 100 kPa, stretchability up to 800%, and resilience up to 98%. Such properties enable these gels to catapult projectiles. Furthermore, these gels achieve a retraction velocity of 16 m s-1 with an acceleration of 4 × 103 m s-2 when released from a stretched state, and these values are comparable to those observed in many biological species during a power amplification process. By utilizing and tuning the simple synthetic strategy used here, these gels can be used in soft robotics, prosthetics, and engineered devices where power amplification is desired.

Paper-Cut Flexible Multifunctional Electronics Using MoS2 Nanosheet.

Art and science represent human creativity and rational thinking, respectively. When the two seemingly opposite fields are intertwined, there is always a life-changing spark. In particular, the integration of ancient traditional Chinese art into the latest electronic devices is always been an unexcavated topic. Fabricating two-dimensional material with a tensile strain less than 3% with an ultimate global stretch has been an important problem that plagues the current flexible electronics field. The current research is limited to material in small scale, and it is always necessary to develop and extend large-sized flexible electronic systems. Here, inspired by the traditional Chinese paper-cut structure, we present a highly deformable multifunctional electronic system based on the MoS2 nanosheet. In this work, we first demonstrate how the traditional paper-cut structure can open the view of flexible electronics. In order to obtain a large area of MoS2 with excellent performance, we use a metal-assisted exfoliation method to transfer MoS2, followed by fabricating a field effect transistor to characterize its excellent electrical properties. Two photodetectors and a temperature sensor are produced with good performance. The mechanical simulation proves that the structure has more advantages in stretchability than other typical paper-cut structures. From the experimental and mechanical point of view, it is proved that the device can work stably under high deformation. We finally show that the device has broad application prospects in highly deformed organs, tissues, and joints. These findings set a good example of traditional Chinese culture to guide innovation in the field of electronic devices.

Applications of Highly Stretchable and Tough Hydrogels.

Stretchable and tough hydrogels have drawn a lot of attention recently. Due to their unique properties, they have great potential in the application in areas such as mechanical sensing, wound healing, and drug delivery. In this review, we will summarize recent developments of stretchable and tough hydrogels in these areas.

Highly Stretchable Micro/Nano Wrinkle Structures for Infrared Stealth Application.

We demonstrate a novel infrared stealth structure consisting of SiO2/TiO2 film, which was manufactured as the highly stretchable triangular wrinkle structures. The triangular wrinkle structures have firstly been transferred to the flexible substrate from the surface of Si-substrate, which was manufactured by the MEMS technology. Then, the infrared reflective film have been manufactured to be the triangular wrinkle structures by depositing the materials (noble metal (Ag or Au) or multilayer oxide (SiO2/TiO2)) on the surface of flexible substrate. Due to the lower reflection effect of curved surface, the infrared reflectivity of these structures has been tuned down to 5%. And, compared to the flat surface, the reflection-to-diffuse ratios improved approximately one order of magnitude. These structures can adapt to the environment by changing the reflectivity of triangular wrinkle structures under stretching. Finally, an Au-modified infrared stealth structure has been fabricated as the array structures, which disappeared and then display by stretching the triangular wrinkle structures at room temperature. It features high reflection-to-diffuse ratios, stable repeatability, low-cost, and easy to manufacture. It may open opportunities for infrared camouflage for military security and surveillance field application.

3D Printing of Highly Stretchable, Shape-Memory, and Self-Healing Elastomer toward Novel 4D Printing.

The three-dimensional (3D) printing of flexible and stretchable materials with smart functions such as shape memory (SM) and self-healing (SH) is highly desirable for the development of future 4D printing technology for myriad applications, such as soft actuators, deployable smart medical devices, and flexible electronics. Here, we report a novel ink that can be used for the 3D printing of highly stretchable, SM, and SH elastomer via UV-light-assisted direct-ink-write printing. An ink containing urethane diacrylate and a linear semicrystalline polymer is developed for the 3D printing of a semi-interpenetrating polymer network elastomer that can be stretched by up to 600%. The 3D-printed complex structures show interesting functional properties, such as high strain SM and SM -assisted SH capability. We demonstrate that such a 3D-printed SM elastomer has the potential application for biomedical devices, such as vascular repair devices. This research paves a new way for the further development of novel 4D printing, soft robotics, and biomedical devices.

Highly Stretchable, Shape Memory Organohydrogels Using Phase-Transition Microinclusions.

Shape memory effect in polymer materials has attracted considerable attention due to its promising applications in a variety of fields. However, shape memory polymers prepared by conventional strategy suffer from a common problem, in which high strain capacity and excellent shape memory behavior cannot be simultaneously achieved. This study reports a general and synergistic strategy to fabricate high-strain and tough shape memory organohydrogels that feature binary cooperative phase. The phase- transition micro-organogels and elastic hydrogel framework act synergistically to provide excellent thermomechanical performance and shape memory effect. During shape memory process, the organohydrogels exhibit high strain capacity, featuring fully recoverable stretching deformation by up to 2600% and compression by up to 85% beneath a load ≈20 times the organohydrogel's weight. Furthermore, owing to the micro-organogel and hydrogel heterostructures, the interfacial tension derived from heterophases dominates the shape recovery of the organohydrogel material. Simple processing and smart surface patterning of the shape memory behavior and multiple shape memory effects can also be realized. Meanwhile, these organohydrogels are also nonswellable in water and oil, which is important for multimedia applications.

Highly Stretchable and UV Curable Elastomers for Digital Light Processing Based 3D Printing.

Stretchable UV-curable (SUV) elastomers can be stretched by up to 1100% and are suitable for digital-light-processing (DLP)-based 3D-printing technology. DLP printing of these SUV elastomers enables the direct creation of highly deformable complex 3D hollow structures such as balloons, soft actuators, grippers, and buckyball electronical switches.