Mechanical robust and highly conductive composite hydrogel reinforced by a combination of cellulose nanofibrils/polypyrrole toward high-performance strain sensor

Conductive hydrogels show promising applications in wearable electronic devices. However, it is still challenging to increase the conductivity as well as the mechanical performance of the conductive hydrogels. In addition, it is more challenging to fabricate ultrathin conductive films with good mechanical strength and high transparency. In this study, a metal‐free flexible conductive hydrogel for flexible wearable strain sensor with high sensitivity is presented. The conductive hydrogel is prepared by polyvinyl alcohol (PVA) templated polymerizing of polypyrrole (PPy) followed by gelating based on the polymerizing and cross‐linking of polyacrylamide (PAAm). The conductive hydrogel is endowed excellent mechanical properties by multiple hydrogen bonds between the interpenetrating network of PVA, PPy, and PAAm. The tensile strength reaches up to 0.2 MPa at 500% and the compression strength reaches up to 1.5 MPa at 90%. It can withstand cyclic loads. The conductivity reaches 0.3 s m−1 and it is sensitive to stretching and compressing. Therefore, strain sensors are prepared based on such hydrogels to make wearable electronic devices, monitoring the subtle and large strains. It is worth noting that the composite material containing PVA has good film‐forming properties. Therefore, ultrathin conductive hydrogel films with high transparency (94.2%), high conductivity (7090 Ω/square) and large‐area are fabricated at low cost.

Highly conductive and tough polyacrylamide/sodium alginate hydrogel with uniformly distributed polypyrrole nanospheres for wearable strain sensors

Waterproof conductive fiber with microcracked synergistic conductive layer for high-performance tunable wearable strain sensor

Flexible sensors are garnering substantial interests for various promising applications, including medical electronics, environmental monitoring, and wearable devices. Developing a flexible sensor with high compliance, high sensitivity, and high reliability through the construction of a novel composite conductive hydrogel based on the synergistic enhancement effect of conductive polymers and metal ions is a remarkable achievement. Herein, an electronic/ionic‐conductive double network hydrogel (polypyrrole (PPy)/carboxymethyl cellulose (CMC)‐Al3+/polyvinyl alcohol (PVA)) with soft compliance, highly conductivity, and stability is presented. Moreover, owing to the synergistic reinforcement effect of the relatively immobilized “islands” of PPy particles and large amounts of movable “bridges” of aluminum ions (Al3+) within the double network hydrogel, the as‐optimized PPy/CMC‐Al3+/PVA composite gels exhibit excellent conductivity (σ = 3.47 ± 0.25 S m−1) and mechanical properties (E = 18.53 ± 0.67 kPa). Furthermore, it has been developed as strain sensors with relatively high linear sensitivity (gauge factor = 2.58) within a broad linearity range (0–400%). It can also be served as a monitoring devices for subtle physiological signals emanating from various parts of the human body. The robust sensor has great potential to be developed as wearable electronic devices and applied in healthcare monitoring fields.

Flexible and wearable hydrogel strain sensors have attracted tremendous attention for applications in human motion and physiological signal monitoring. However, it is still a great challenge to develop a hydrogel strain sensor with certain mechanical properties and tensile deformation capabilities, which can be in conformal contact with the target organ and also have self-healing properties, self-adhesive capability, biocompatibility, antibacterial properties, high strain sensitivity, and stable electrical performance. In this paper, an ionic conductive hydrogel (named PBST) is rationally designed by proportionally mixing polyvinyl alcohol (PVA), borax, silk fibroin (SF), and tannic acid (TA). SF can not only be a reinforcement to introduce an energy dissipation mechanism into the dynamically cross-linked hydrogel network to stabilize the non-Newtonian behavior of PVA and borax but it can also act as a cross-linking agent to combine with TA to reduce the dissociation of TA on the hydrogel network, improving the mechanical properties and viscoelasticity of the hydrogel. The combination of SF and TA can improve the self-healing ability of the hydrogel and realize the adjustable viscoelasticity of the hydrogel without sacrificing other properties. The obtained hydrogel has excellent stretchability (strain > 1000%) and shows good conformal contact with human skin. When the hydrogel is damaged by external strain, it can rapidly self-repair (mechanical and electrical properties) without external stimuli. It shows adhesiveness and repeatable adhesiveness to different materials (steel, wood, PTFE, glass, iron, and cotton fabric) and biological tissues (pigskin) and is easy to peel off without residue. The obtained PBST conductive hydrogel also has a wide strain-sensing range (>650%) and reliable stability. The hydrogel adhered to the skin surface can monitor large strain movements such as in finger joints, wrist joints, knee joints, and so on and detect swallowing, smiling, facial bulging and calming, and other micro-deformation behaviors. It can also distinguish physical signals such as light smile, big laugh, fast and slow breathing, and deep and shallow breathing. Therefore, the PBST conductive hydrogel material with multiple synergistic functions has great potential as a flexible wearable strain sensor. The PBST hydrogel has antibacterial properties and good biocompatibility at the same time, which provides a safety guarantee for it as a flexible wearable strain sensor. This work is expected to provide a new way for people to develop ideal wearable strain sensors.

Skin-mimicking strategy to fabricate strong and highly conductive anti-freezing cellulose-based hydrogels as strain sensors

Flexible strain sensors have aroused widespread concern due to their potential applications in detecting human motion and health. Carbon-based materials are surpassing candidate materials for flexible strain sensors with superior performances, because of their outstanding electrical conductivity, lightweight and flexibility, and excellent stability. In order to satisfy the detecting requirements for different strain forms in practical applications, various types of strain sensors based on carbon materials have been designed and prepared, including tensile, pressure, bending, torsion, and multiplex strain sensors. Herein, the latest advances in the preparation of flexible carbon-based strain sensors are reviewed according to the strain types. Furthermore, the potential applications and existing challenges of sensors in the field of human motion and physiological information detection are summarized. This review aims to provide some references for further exploitation of high-performance flexible carbon-based strain sensors.

Transparent and conductive amino acid-tackified hydrogels as wearable strain sensors

Stretchable, transparent, self-adhesive, anti-freezing and ionic conductive nanocomposite hydrogels for flexible strain sensors

Flexible strain sensors have a wide range of applications, such as human motion monitoring, wearable electronic devices, and human-computer interactions, due to their good conformability and sensitive deformation detection. To overcome the internal stress problem of solid sensing materials during deformation and prepare small-sized flexible strain sensors, it is necessary to choose a more suitable sensing material and preparation technology. We report a simple and high-performance flexible strain sensor based on liquid metal nanoparticles (LMNPs) on a polyimide substrate. The LMNPs were assembled using the femtosecond laser direct writing technology to form liquid metal microwires. A wearable strain sensor from the liquid metal microwire was fabricated with an excellent gauge factor of up to 76.18, a good linearity in a wide sensing range, and a fast response/recovery time of 159 ms/120 ms. Due to these extraordinary strain sensing performances, the strain sensor can monitor facial expressions in real time and detect vocal cord vibrations for speech recognition.

Ultra-stretchable and anti-freezing ionic conductive hydrogels as high performance strain sensors and flexible triboelectric nanogenerator in extreme environments

Ionic conductive hydrogels have attracted increasing research interest in flexible electronics. However, the limited resilience and poor fatigue resistance of current ionic hydrogels significantly restrict their practical application. Herein, an urushiol-based ionic conductive double network hydrogel (PU/PVA-Li) was developed by one-pot thermal initiation polymerization assisted with freeze-thaw cycling and subsequent LiCl soaking. Such a PU/PVA-Li hydrogel comprises a primary network of covalently crosslinked polyurushiol (PU) and a secondary network formed by physically crosslinked poly(vinyl alcohol) (PVA) through crystalline regions. The obtained PU/PVA-Li hydrogel demonstrates exceptional mechanical properties, including ultrahigh strength (up to 3.4 MPa), remarkable toughness (up to 1868.6 kJ/m3), and outstanding fatigue resistance, which can be attributed to the synergistic effect of the interpenetrating network structure and dynamic physical interactions between PU and PVA chains. Moreover, the incorporation of LiCl into the hydrogels induces polymer chain contraction via ionic coordination, further enhancing their mechanical strength and resilience, which also impart exceptional ionic conductivity (2.62 mS/m) to the hydrogels. Based on these excellent characteristics of PU/PVA-Li hydrogel, a high-performance flexible strain sensor is developed, which exhibits high sensitivity, excellent stability, and reliability. This PU/PVA-Li hydrogel sensor can be effectively utilized as a wearable electronic device for monitoring various human joint movements. This PU/PVA-Li hydrogel sensor could also demonstrate its great potential in information encryption and decryption through Morse code. This work provides a facile strategy for designing versatile, ultrastrong, and tough ionic conductive hydrogels using sustainable natural extracts and biocompatible polymers. The developed hydrogels hold great potential as promising candidate materials for future flexible intelligent electronics.

Superhydrophobic flexible strain sensors have great application value in the fields of personal health monitoring, human motion detection, and soft robotics due to their good flexibility and high sensitivity. However, complicated preparation processes and costly processing procedures have limited their development. To overcome these limitations, in this work we develop a facile and low-cost method for fabricating superhydrophobic flexible strain sensor via spraying carbon black (CB) nanoparticles dispersed in a thermoplastic elastomer (SEBS) solution on a polydimethylsiloxane (PDMS) flexible substrate. The prepared strain sensor had a large water contact angle of 153 ± 2.83° and a small rolling angle of 8.5 ± 1.04°, and exhibited excellent self-cleaning property. Due to the excellent superhydrophobicity, aqueous acid, salt, and alkali could quickly roll off the flexible strain sensor. In addition, the sensor showed excellent sensitivity (gauge factor (GF) of 5.4–7.35), wide sensing ranges (stretching: over 70%), good linearity (three linear regions), low hysteresis (hysteresis error of 4.8%), and a stable response over 100 stretching-releasing cycles. Moreover, the sensor was also capable of effectively detecting human motion signals like finger bending and wrist bending, showing promising application prospects in wearable electronic devices, personalized health monitoring, etc.

Highly stretchable, self-healing, and strain-sensitive based on double-crosslinked nanocomposite hydrogel

High-performance strain sensor for detection of human motion and subtle strain by facile fabrication