Hydrogel-based conductive materials for smart wearable devices have attracted increasing attention due to their excellent flexibility, versatility, and outstanding biocompatibility. This review presents the recent advances in multifunctional conductive hydrogels for electronic devices. First, conductive hydrogels with different components are discussed, including pure single network hydrogels based on conductive polymers, single network hydrogels with additional conductive additives (i.e., nanoparticles, nanowires, and nanosheets), double network hydrogels based on conductive polymers, and double network hydrogels with additional conductive additives. Second, conductive hydrogels with a variety of functionalities, including self-healing, super toughness, self-growing, adhesive, anti-swelling, antibacterial, structural color, hydrophobic, anti-freezing, shape memory and external stimulus responsiveness are introduced in detail. Third, the applications of hydrogels in flexible devices are illustrated (i.e., strain sensors, supercapacitors, touch panels, triboelectric nanogenerator, bioelectronic devices, and robot). Next, the current challenges facing hydrogels are summarized. Finally, an imaginative but reasonable outlook is given, which aims to drive further development in the future.

Recent advances in conductive hydrogels: classifications, properties, and applications.

A Conductive Hydrogel based on Nature Polymer Agar with Self-healing Ability and Stretchability for Flexible Sensors

Underwater adhesion plays an essential role in soft electronics for the underwater interface. Although hydrogel-based electronics are of great interest, because of their versatility, water molecules prevent hydrogels from adhering to substrates, thus bottlenecking further applications. Herein, inspired by the barnacle proteins, MXene/PHMP hydrogels with strong repeatable underwater adhesion are developed through the random copolymerization of 2-phenoxyethyl acrylate, 2-methoxyethyl acrylate, and N-(2-hydroxyethyl) acrylamide with the presence of MXene nanosheets. The hydrogels are mechanically tough (elastic modulus of 32 kPa, fracture stress of 0.11 MPa), and 2-phenoxyethyl acrylate (PEA) with aromatic groups endows the hydrogel with nonswelling property and prevents water molecules from invading the adhesive interface, rendering the hydrogels an outstanding adhesive behavior toward various substrates (including glass, iron, polyethylene terephthalate (PET), porcine). Besides, dynamic physical interactions allow for instant and repeatable underwater adhesion. Furthermore, the MXene/PHMP hydrogels exhibit a high conductivity (0.016 S/m), fast responsiveness, and superior sensitivity as a strain sensor (gauge factor = 7.17 at 200%-500% strain) and pressure sensor (0.63 kPa-1 at 0-70 kPa). The underwater applications of bionic hydrogel-based sensors have been demonstrated, such as human motion, pressure sensing, and holding objects. It is anticipated that the instant and repeatable underwater adhesive hydrogel-based sensors extend the underwater applications of hydrogel electronics.

Bio-Inspired Instant Underwater Adhesive Hydrogel Sensors.

Robust superhydrophobic wearable piezoelectric nanogenerators for self-powered body motion sensors

Flexible strain sensors are promising candidates for intelligent wearable devices. Among previous studies, although crack-based sensors have attracted a lot of attention due to their ultrahigh sensitivity, large strain usually causes fractures in the conductive paths. Because of the unstable crack structure, the tradeoff between sensitivity and workable strain range is still a challenge. As carbon nanotubes (CNTs) and silver nanowires (AgNWs) can form a strong interface with the thermoplastic substrate and strengthen the conductive network by capillary force during water evaporation, CNTs and AgNWs were deposited on electrospun TPU fiber mats via vacuum-assisted filtration in this work. The prestretching treatment constructed a microcrack structure that endowed the sensor with the combined characteristics of a wide working range (0~171% strain), ultrahigh sensitivity (a gauge factor of 691 within 0~102% strain, ~2 × 104 within 102~135% strain, and >11 × 104 within 135~171% strain), a fast response time (~65 ms), small hysteresis, and superior durability (>2000 cycles). Subsequently, the sensing mechanism of the sensor was studied. Distributed microcrack propagation based on the "island-bridge" structure was explained in detail, and its influence on the strain-sensing behavior of the sensor was analyzed. Finally, the sensor was assembled to monitor various vibration signals and human motions, demonstrating its potential applications in the fields of electronic skin and human health monitoring. 

/pdf/an-ultrasensitive-and-stretchable-strain-sensor-based-on-a-m9pi78e2.pdf

An ultrasensitive and stretchable strain sensor based on a microcrack structure for motion monitoring

Conductive hydrogels are promising multifunctional materials for wearable sensors, but their practical applications require combined properties that are difficult to achieve. Herein, we developed a flexible wearable sensor with double-layer structure based on conductive composite hydrogel, which included the outer layer of silicone elastomer (Ecoflex)/silica microparticle composite film and the inner layer of P(AAm-co-HEMA)-MXene-AgNPs hydrogel. Through covalently cross-linking silicone elastomer on the surface of the hydrogel polymer, we bonded a thin Ecoflex film (100 μm) on the P(AAm-co-HEMA)-MXene-AgNPs hydrogel with robust interface, which can easily adhere to the Ecoflex/SiO2 microparticle composite film by silicone glue. The Ecoflex/SiO2 microparticle composite film endows the strain wearable sensor with superhydrophobic function that could maintain the stability under stretching or bending. Moreover, it can effectively resist the interference of water droplets and water flow. The P(AAm-co-HEMA)-MXene-AgNPs hydrogel exhibits outstanding antibacterial activity to inhibit Staphylococcus aureus, Escherichia coli, and even drug-resistant Escherichia coli. In addition, the flexible wearable sensor exhibited good self-adhesive performance by changing the reaction temperature of hydrogel and can adhere strongly onto various materials. The conductive composite hydrogel reported in this work contributes an innovative strategy for the preparation of multifunctional flexible wearable sensor.

Antiliquid-Interfering, Antibacteria, and Adhesive Wearable Strain Sensor Based on Superhydrophobic and Conductive Composite Hydrogel.

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Antiliquid-Interfering, Antibacteria, and Adhesive Wearable Strain Sensor Based on Superhydrophobic and Conductive Composite Hydrogel.