Harmonizing Elastic Modulus and Dielectric Constant of Elastomers for Improved Pressure Sensing Performance.

Enhancing the sensitivity of capacitive pressure sensors through microstructure design may compromise the reliability of the device and rely on intricate manufacturing processes. It is an effective way to solve this issue by balancing the intrinsic properties (elastic modulus and dielectric constant) of the dielectric layer materials. Here, we introduce a liquid metal (LM) hybrid elastomer prepared by a chain-extension-free polyurethane (PU) and LM. The synergistic strategies of extender-free and LM doping effectively reduce the elastic modulus (7.6 ± 0.2-2.1 ± 0.3 MPa) and enhance the dielectric constant (5.12-8.17 @1 kHz) of LM hybrid elastomers. Interestingly, the LM hybrid elastomer combines reprocessability, recyclability, and photothermal conversion. The obtained flexible pressure sensor can be used for detecting hand and throat muscle movements, and high-precision speech recognition of seven words has been using a convolutional neural network (CNN) in deep learning. This work provides an idea for designing and manufacturing wearable, recyclable, and intelligent control pressure sensors.

Spider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties.

Ideal hydrogel fibers with high toughness and environmental tolerance are indispensable for their long-term application in flexible electronics as actuating and sensing elements. However, current hydrogel fibers exhibit poor mechanical properties and environmental instability due to their intrinsically weak molecular (chain) interactions. Inspired by the multilevel adjustment of spider silk network structure by ions, bionic hydrogel fibers with elaborated ionic crosslinking and crystalline domains are constructed. Bionic hydrogel fibers show a toughness of 162.25 ± 21.99 megajoules per cubic meter, comparable to that of spider silks. The demonstrated bionic structural engineering strategy can be generalized to other polymers and inorganic salts for fabricating hydrogel fibers with broadly tunable mechanical properties. In addition, the introduction of inorganic salt/glycerol/water ternary solvent during constructing bionic structures endows hydrogel fibers with anti-freezing, water retention, and self-regeneration properties. This work provides ideas to fabricate hydrogel fibers with high mechanical properties and stability for flexible electronics.

Bilayer Hydrogel Actuators with High Mechanical Properties and Programmable Actuation via the Synergy of Double-Network and Synchronized Ultraviolet Polymerization Strategies.

Bilayer hydrogel actuators, consisting of an actuating layer and a functional layer, show broad applications in areas such as soft robotics, artificial muscles, drug delivery and tissue engineering due to their inherent flexibility and responses to stimuli. However, to achieve the compatibility of good stimulus responses and high mechanical properties of bilayer hydrogel actuators is still a challenge. Herein, based on the double-network strategy and using the synchronous ultraviolet (UV) polymerization method, an upper critical solution temperature (UCST)-type bilayer hydrogel actuator was prepared, which consisted of a poly(acrylamide-co-acrylic acid)[MC] actuating layer and an agar/poly(N-hydroxyethyl acrylamide-co-methacrylic acid)[AHA] functional layer. The results showed that the tensile stress/strain of the bilayer hydrogel actuator was 1161.21 KPa/222.07%. In addition, the UCST of bilayer hydrogels was ~35 °C, allowing the bilayer hydrogel actuator to be curled into an "◎" shape, which could be unfolded when the temperature was 65 °C, but not at a temperature of 5 °C. Furthermore, hydrogel actuators of three different shapes were designed, namely "butterfly", "cross" and "circle", all of which demonstrated good actuating performances, showing the programmable potential of bilayer hydrogels. Overall, the bilayer hydrogels prepared using double-network and synchronous UV polymerization strategies realized the combination of high mechanical properties with an efficient temperature actuation, which provides a new method for the development of bilayer hydrogel actuators.

Continuous Spinning of High-Tough Hydrogel Fibers for Flexible Electronics by Using Regional Heterogeneous Polymerization.

Hydrogel fibers have attracted substantial interest for application in flexible electronics due to their ionic conductivity, high specific surface area, and ease of constructing multidimensional structures. However, universal continuous spinning methods for hydrogel fibers are yet lacking. Based on the hydrophobic mold induced regional heterogeneous polymerization, a universal self-lubricating spinning (SLS) strategy for the continuous fabrication of hydrogel fibers from monomers is developed. The universality of the SLS strategy is demonstrated by the successful spinning of 10 vinyl monomer-based hydrogel fibers. Benefiting from the universality of the SLS strategy, the SLS strategy can be combined with pre-gel design and post-treatment toughening to prepare highly entangled polyacrylamide (PAM) and ionic crosslinked poly(acrylamide-co-acrylic acid)/Fe3+ (W-PAMAA/Fe3+ ) hydrogel fibers, respectively. In particular, the W-PAMAA/Fe3+ hydrogel fiber exhibited excellent mechanical properties (tensile stress > 4 MPa, tensile strain > 400%) even after 120 days of swelling in the pH of 3-9. Furthermore, owing to the excellent multi-faceted performance and one-dimensionality of W-PAMAA/Fe3+ hydrogel fibers, flexible sensors with different dimensions and functions can be constructed bottom-up, including the one-dimensional (1D) strain sensor, two-dimensional (2D) direction sensor, three-dimensional (3D) pressure sensor, and underwater communication sensor to present the great potential of hydrogel fibers in flexible electronics.

Smart Antifreeze Hydrogels with Abundant Hydrogen Bonding for Conductive Flexible Sensors.

Recently, flexible sensors based on conductive hydrogels have been widely used in human health monitoring, human movement detection and soft robotics due to their excellent flexibility, high water content, good biocompatibility. However, traditional conductive hydrogels tend to freeze and lose their flexibility at low temperature, which greatly limits their application in a low temperature environment. Herein, according to the mechanism that multi-hydrogen bonds can inhibit ice crystal formation by forming hydrogen bonds with water molecules, we used butanediol (BD) and N-hydroxyethyl acrylamide (HEAA) monomer with a multi-hydrogen bond structure to construct LiCl/p(HEAA-co-BD) conductive hydrogel with antifreeze property. The results indicated that the prepared LiCl/p(HEAA-co-BD) conductive hydrogel showed excellent antifreeze property with a low freeze point of -85.6 °C. Therefore, even at -40 °C, the hydrogel can still stretch up to 400% with a tensile stress of ~450 KPa. Moreover, the hydrogel exhibited repeatable adhesion property (~30 KPa), which was attributed to the existence of multiple hydrogen bonds. Furthermore, a simple flexible sensor was fabricated by using LiCl/p(HEAA-co-BD) conductive hydrogel to detect compression and stretching responses. The sensor had excellent sensitivity and could monitor human body movement.

A Review of Conductive Hydrogel Used in Flexible Strain Sensor.

Hydrogels, as classic soft materials, are important materials for tissue engineering and biosensing with unique properties, such as good biocompatibility, high stretchability, strong adhesion, excellent self-healing, and self-recovery. Conductive hydrogels possess the additional property of conductivity, which endows them with advanced applications in actuating devices, biomedicine, and sensing. In this review, we provide an overview of the recent development of conductive hydrogels in the field of strain sensors, with particular focus on the types of conductive fillers, including ionic conductors, conducting nanomaterials, and conductive polymers. The synthetic methods of such conductive hydrogel materials and their physical and chemical properties are highlighted. At last, challenges and future perspectives of conductive hydrogels applied in flexible strain sensors are discussed.