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Since hydrogels are conductive, easily engineered, and sufficiently flexible to imitate the mechanical properties of human skin, they are seen as potential options for wearable strain sensors. However, it is still a great challenge to prepare a hydrogel through simple and straightforward methods that integrate excellent stretchability, ionic conductivity, toughness, self-adhesion, and self-healing. Herein, an acrylamide/3-acrylamide phenylboronic acid cross-linked network is modified to produce a semi-interpenetrating cross-linked hydrogel in just one easy step by adding starch. The prepared hydrogel contains dynamic boronic ester bonds and hydrogen bonds, which endow the exceptional stretchability (5769-13,976 %, 20-50 wt%), ideal transmittance (>90 %), self-adhesiveness (0.636 ± 0.060 kPa, 30 wt%), and self-healing properties. Notably, the self-healing process is completed instantly, achieving a healing strength of up to 81.21 %. Additionally, the aforementioned hydrogel exhibits a broad working strain range (≈ 500 %) and high sensitivity (gauge factor = 1.99) as a strain sensor, allowing it to record and track human actions precisely. This work provides a novel approach to synthesizing hydrogels with optimal overall mechanical characteristics, with the potential to facilitate the development of wearable strain sensing system based on hydrogels for real-world applications., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Yanyan Li reports financial support was provided by Youth Science Foundation of Shanxi Province (202203021222012). Jian Zhang reports financial support was provided by Natural Science Foundation of Shanxi Province (20210302123458). If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Fibrous strain sensing materials with both high sensitivity and high linearity are of significant importance for wearable sensors, yet they still face great challenges. Herein, a photo-spun reaction encapsulation strategy is proposed for the continuous fabrication of fibrous strain sensor materials (AMGF) with a core-sheath structure. Metallogels (MOGs) formed by bacterial cellulose (BC) nanofibers and Ag nanoparticles (AgNPs), and thermoplastic elastomers (TPE) are employed as the core and sheath, respectively. The in situ ultraviolet light reduction of Ag + ensured AgNPs to maintain the interconnections between the BC nanofibers and form electron conductive networks (0.31 S m -1 ). Under applied strain, the BC nanofibers experience separation, bringing AMGF a high sensitivity (gauge factor 4.36). The concentration of free ions in the MOGs uniformly varies with applied deformation, endowing AMGF with high linearity and a goodness-of-fit of 0.98. The sheath TPE provided AMGF sensor with stable working life (>10 000 s). Furthermore, the AMGF sensors are demonstrated to monitor complex deformations of the dummy joints in real-time as a wearable sensor. Therefore, the fibrous hybrid conductive network fibers fabricated via the photo-spun reaction encapsulation strategy provide a new route for addressing the challenge of achieving both high sensitivity and high linearity., (© 2023 Wiley-VCH GmbH.)

Addressing the critical requirement for real-time monitoring of tumor progression in cancer care, this study introduces an innovative wearable platform. This platform employs a thermoplastic polyurethane (TPU) film embedded with hafnium oxide nanoparticles (HfO 2 NPs) to facilitate dynamic tracking of tumor growth and regression in real time. Significantly, the synthesized HfO 2 NPs exhibit promising characteristics as effective sonosensitizers, holding the potential to efficiently eliminate cancer cells through ultrasound irradiation. The TPU-HfO 2 film, acting as a dielectric elastomer (DE) strain sensor, undergoes proportional deformation in response to changes in the tumor volume, thereby influencing its electrical impedance. This distinctive behavior empowers the DE strain sensor to continuously and accurately monitor alterations in tumor volume, determining the optimal timing for initiating HfO 2 NP treatment, optimizing dosages, and assessing treatment effectiveness. Seamless integration with a wireless system allows instant transmission of detected electrical impedances to a smartphone for real-time data processing and visualization, enabling immediate patient monitoring and timely intervention by remote medical staff. By combining the dynamic tumor monitoring capabilities of the TPU-HfO 2 film with the sonosensitizer potential of HfO 2 NPs, this approach propels cancer care into the realm of telemedicine, representing a significant advancement in patient treatment.

Regenerated silk fibroin (RSF) hydrogels have been extensively studied in the fields of biomedicine and wearable devices in recent years due to their outstanding biocompatibility. However, the pure RSF hydrogels usually exhibited frangibility and low ductility, limiting their application in many aspects severely. Herein, we demonstrate a tough RSF/poly (N, N-dimethylallylamine) hydrogel with semi-interpenetrating network, which possesses good mechanical properties with high stretchability (ε b  = 900%), tensile strength (σ b  = 101.7 kPa), toughness (W f  = 516.7 kJ/m 3 ) and tearing fracture energy (T = 407.3 J/m 2 ). Besides, the gels show low residual strain in the cyclic tests and rapid self-recovery (80% toughness recovery within 5 min with the maximum strain of 400%). Moreover, the gels also show high ionic conductivity due to the incorporation of the NaCl and the hydrogel can act as an ideal candidate for strain sensor with high sensitivity (GF = 1.84), admirable linearity, and good durability (1000 cycles with the strain of 100%). When used as a wearable strain sensor for monitoring human movements, it also can detect small and large deformations with high sensitivity. It is expected that this work can provide a new strategy for the fabrication of smart RSF-based hydrogels and expand their application in multiple scenarios., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Conductive hydrogels as wearable devices meet the basic demands of mechanical flexibility and smart sensing. However, achieving anti-freeze property in conductive hydrogels is still challengeable. Here, a novel anti-freezing system based on ice structuring proteins and CaCl 2 was introduced to enable a conductive hydrogel with low-temperature adaptability. Both formation of ice nuclei and ice growth of the hydrogel at sub-zero temperature could be inhibited. Supported by the anti-freeze system, the hydrogel revealed good flexibility (890% at -20 °C), recovery and conductivity (0.50 S/m at -20 °C) at both room temperature and sub-zero temperature. The low-temperature adaptability enabled the hydrogel to be used as strain and temperature sensors at both room temperature and sub-zero temperature. The anti-freeze system in this work is expected to open up a new avenue to promote the conductive hydrogel with low-temperature adaptability., (Copyright © 2021. Published by Elsevier B.V.)

Adaptability could meet basic technological application requirements. Therefore, a hydrogel-based transducer with durable adhesion, ultrahigh toughness, and super resilience was highly demanded. Here, a skin-like hydrogel transducer was successfully prepared through introducing carboxymethyl chitosan and sodium caseinate into a polyacrylamide hydrogel system. In addition, the polyacrylamide-sodium casein-carboxymethyl chitosan (PAAM-SC-CC) hydrogel has strong mechanical properties and excellent mechanical flexibility, largely due to the adequate energy dissipation mechanism. Surprisingly, the PAAM-SC-CC hydrogel exhibited stable and reproducible adhesion to various solid substrates and the human skin. Due to abundant free ions driven from sodium caseinate, the PAAM-SC-CC hydrogel could maintain stable and sensitive ionic conductivity without adding additional fillers. Experiments have proved that it can be applied to the field of human motion monitoring with complex signals. Therefore, the PAAM-SC-CC hydrogel sensor could monitor human movement in different strain ranges, including throat movement and joint extension. Such a flexible hydrogel-based transducer with various properties is conceivable to broaden the application field of bioelectrodes, human machines, personalized medical health fields, etc.

Hypothesis: Flexible and wearable hydrogel strain sensors have attracted significant attention for human activity monitoring and electronic skins. However, it remains a great challenge to develop an integrated hydrogel strain sensor showing intrinsic adhesive performances, tunable mechanical and high strain-sensitive properties. Marine mussels show a superior capacity to adhere to various substrates (including organic and inorganic), while polycaprolactone (PCL) can be easily modified into crosslinkers with different degrees of functionality (bi-, tri-, and quadri-functional groups) to control the crosslinking density. Therefore, the developed mussel-inspired 3,4-dihydroxyphenyl-l-alanine acrylamide-polycaprolactone (l-DMA-PCL) hydrogels could address these issues and serve as the potential wearable strain sensors for biomaterials and healthcare monitoring., Experiments: l-DMA monomers were successfully crosslinked by functionalized PCL (bi-, tri-, and quadri-functional) using UV light (wavelength ~ 365 nm) to prepare the l-DMA-PCL hydrogel. Adhesive behaviors, tunable mechanical properties and strain sensing performances of the l-DMA-PCL hydrogels were systematically studied., Findings: The l-DMA-PCL hydrogel exhibited reversible adhesion to various material substrates (including steel, aluminum, ceramics, poly(ethylene terephthalate) (PET), wood, rubber, even for polypropylene (PP) and polytetrafluoroethylene (PTFE)) as well as skin. Moreover, the mechanical properties (stress: 50.2-72.4 KPa, strain: 700-1140%, Young's modulus: 8.6-14.8 KPa, and toughness: 16.4-53.6 KJ/m 3 ) of the hydrogels could be readily tuned by the modulation of functionality degree (bi-, tri-, and quadri-functional) of PCL. Intriguingly, the hydrogel-based wearable strain sensor showing high conductivity (0.0550 S/cm) and sensitive responses to both large (e.g., joint bending) and subtle human motions (e.g., frowning and speaking). Based on these achievements, this work provides new insights into the development of hydrogel with adhesiveness, controllable mechanical performance and high strain sensitivity as a flexible and wearable hydrogel strain sensors., Competing Interests: Declaration of Competing Interest The authors declare no known conflicts of interest to this work., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Owning to the viscoelastic properties, good biocompatibility and high strain sensitivity, choline chloride-based deep eutectic solvent (DES) hydrogels have been considered to be promising wearable strain sensors for human motion. However, traditional hydrogels are far away from the wearable strain sensor applications caused by their unsatisfied conductivity and weak mechanical properties. Herein, the strategy for functional ionic inorganic/organic interpenetrating (IPN) hydrogels preparation by cyclic freezing/thawing method was successfully developed. Polyvinyl alcohol (PVA) was proposed to dissolve in choline chlorede-based DES as hydrogel matrix for the first time. Encouragingly, the obtained DES/PVA/CNCs/g-C 3 N 4 hydrogel (choline chloride with glucose) exhibits excellent mechanical properties, included excellent tensile strength (≈ 2.55 MPa), high elongation (≈1200 %) and satisfactory tensile modulus (≈3.65 MPa). Interestingly, the thermal diffusivity (the maximum value was 0.675 W/mK) and conductivity (the maximum value was 0.18 mm 2 /s) of the DES-hydrogels were successfully achieved through adding graphitic-like nitride nanosheet (g-C 3 N 4 ) and sustainable cellulose nanocrystalline (CNCs). These enhancements were attributed to the synergistic interactions of powerful hydrogen bonding among DES, CNCs, g-C 3 N 4 and PVA chains. More importantly, the as-prepared hydrogels have the potential as a human motion sensor to accurately in-situ detect human activities on the fingers, wrists, elbows and knee joints. Those hydrogel-type strain sensors with flexibility, excellent mechanical properties, self-recovery, good heat transfer, and electrical conductivity have broad application prospects in the fields of intelligent robot, bionic prostheses, and human care areas., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Conductive hydrogels have shown great potential in the field of flexible strain sensors. However, their application is greatly limited due to the low conductivity and poor mechanical properties at subzero temperatures. Herein, an ultrastretchable, tough, antifreezing, and conductive cellulose hydrogel was fabricated by grafting acrylonitrile and acrylamide copolymers onto the cellulose chains in the presence of zinc chloride using ceric ammonium nitrate as the initiator. The resulting hydrogel exhibited ultrastretchability (1730%), excellent tensile strength (160 kPa), high elasticity (90%), good toughness (1074.7 kJ/m 3 ), and fatigue resistance property due to the existence of dipole-dipole and multiple hydrogen-bonding interactions on the hydrogel network. In addition, the introduced zinc chloride endowed the cellulose-based hydrogel with remarkable electric conductivity (1.54 S/m) and excellent antifreezing performance (-33 °C). Finally, the hydrogel showed high sensitivity and stability to monitor human activities. In summary, this work presented a facile strategy to construct conductive hydrogel with excellent antifreezing and mechanical properties simultaneously, which showed great potential for wearable strain sensors.

The demand for stretchable, flexible, and wearable multifunctional devices based on conductive nanomaterials is rapidly increasing considering their interesting applications including human motion detection, robotics, and human-machine interface. There still exists a great challenge to manufacture stretchable, flexible, and wearable devices through a scalable and cost-effective fabrication method. Herein, we report a simple method for the mass production of electrically conductive textiles, made of cotton and wool, by hybridization of graphene nanoplatelets and carbon black particles. Conductive textiles incorporated into a highly elastic elastomer are utilized as highly stretchable and wearable strain sensors and heaters. The electromechanical characterizations of our multifunctional devices establish their excellent performance as wearable strain sensors to monitor various human motions, such as finger, wrist, and knee joint movements, and to recognize sound with high durability. Furthermore, the electrothermal behavior of our devices shows their potential application as stretchable and wearable heaters working at a maximum temperature of 103 °C powered with 20 V.