Applying conductive hydrogels in electronic skin, health monitoring, and wearable devices has aroused great research interest. Yet, it remains a significant challenge to prepare conductive hydrogels simultaneously with superior mechanical, self-recovery, and conductivity performance. Herein, a dual ionically cross-linked double network (DN) hydrogel is fabricated based on K+ and Fe3+ ion cross-linked κ-carrageenan (κ-CG) and Fe3+ ion cross-linked poly(sodium acrylate-co-acrylamide) P(AANa-co-AM). Benefiting from the abundance of hydrogen bonds and metal coordination bonds, the conductive hydrogel has excellent mechanical properties (fracture strain up to 1420 %, fracture stress up to 2.30 MPa, and toughness up to 20.63 MJ/m3) and good self-recovery performance (the recovery rate of the toughness can reach 85 % after waiting for 1 h). Meanwhile, due to the introduction of dual metal ions of K+ and Fe3+, the ionic conductivity of conductive hydrogel is up to 1.42 S/m. Furthermore, the hydrogel strain sensor has good sensitivity with a gauge factor (GF) of 2.41 (0-100 %). It can be a wearable sensor that monitors different human motions, such as sit-ups. This work offers a new synergistic strategy for designing a hydrogel strain sensor with high mechanical, self-recovery, and conductive properties.

BACKGROUND: Mechanical stresses incurred during post-harvest fruit storage and transportation profoundly impact decay and losses. Currently, the monitoring of mechanical forces is primarily focused on vibrational forces experienced by containers and vehicles and impact forces affecting containers. However, the detection of compressive forces both among interior fruit and between fruit and packaging surfaces remains deficient. Hence, conformable materials capable of sensing compressive stresses are necessary.
OBJECTIVE: In the present study, a triple-network-reinforced PSA/LiCl/CCN@AgNP conductive hydrogel was synthesized for compression force detection on fruit surfaces based on changes in intrinsic impedance under mechanical loading.
METHODS: The conductive hydrogel was characterized in terms of its adhesion, mechanics, frost resistance, water retention, conductivity, mechanical force-sensing properties, and feasibility for monitoring mechanical forces. Then, a portable complex impedance recorder was developed to interface with the conductive hydrogel and its mechanical force sensing ability was evaluated.
RESULTS: Beyond its inherent conductivity, the hydrogel exhibited notable pressure sensitivity within the strain range of 1 % to 80 %. The conductive hydrogel also demonstrated a commendable adhesion property, favorable tensile property (580 % elongation at break), substantial compressive strength and durability, and a long-term water retention capability. After exposure to -20 °C for 96 h, the hydrogel maintained its mechanical strength, affirming its anti-freezing property. In addition, a portable complex impedance recorder with sustained signal measurement stability was developed to quantitatively acquire the hydrogel resistance changes in response to compression forces. Finally, the effectiveness of the conductive hydrogel for sensing compression force on the surface of apple fruits was validated.
CONCLUSIONS: The conductive hydrogel holds promise for applications in smart packaging, wherein it can detect crucial mechanical stress on fruit, convert it into electrical signals, and further transmit these signals to the cloud, thereby enabling the real-time sensing of mechanical forces experienced by fruits and enhancing post-harvest fruit loss management.

Skin-electronic interfaces have broad applications in fields such as diagnostics, therapy, health monitoring, and smart wearables. However, they face various challenges in practical use. For instance, in wet environments, the cohesion of the material may be compromised, and under dynamic conditions, maintaining conformal adhesion becomes difficult, leading to reduced sensitivity and fidelity of electrical signal transmission. The key scientific issue lies in forming a stable and tight mechanical-electronic coupling at the tissue-electronic interface. Here, inspired by octopus sucker structures and snail mucus, we propose a strategy for hydrogel skin-electronic interfaces based on multi-coupled bioinspired adhesion and introduce an ultrasound (US)-mediated interfacial toughness enhancement mechanism. Ultimately, using digital light processing micro-nano additive manufacturing technology (DLP 3D), we have developed a multifunctional, diagnostic-therapeutic integrated patch (PAMS). This patch exhibits moderate water swelling properties, a maximum deformation of up to 460 %, high sensitivity (GF=4.73), and tough and controllable bioadhesion (shear strength increased by 109.29 %). Apart from outstanding mechanical and electronic properties, the patch also demonstrates good biocompatibility, anti-bacterial properties, photothermal properties, and resistance to freezing at -20°C. Experimental results show that this skin-electronic interface can sensitively monitor temperature, motion, and electrocardiogram signals. Utilizing a rat frostbite model, we have demonstrated that this skin-electronic interface can effectively accelerate the wound healing process as a wound patch. This research offers a promising strategy for improving the performance of bioelectronic devices and personalized diagnostics and therapeutics in the future. STATEMENT OF SIGNIFICANCE: Establishing stable and tight mechanical-electronic coupling at the tissue-electronic interface is essential for the diverse applications of bioelectronic devices. This study aims to develop a multifunctional, diagnostic-therapeutic integrated hydrogel skin-electronic interface patch with enhanced interfacial toughness. The patch is based on a multi-coupled bioinspired adhesive-enhanced mechanism, allowing for personalized 3D printing customization. It can be used as a high-performance diagnostic-therapeutic sensor and effectively promote frostbite wound healing. We anticipate that this research will provide new insights for constructing the next generation of multifunctional integrated high-performance bioelectronic interfaces.

Atopic dermatitis is a chronic, inflammation skin disease that remains a major public health challenge. The current drug-loading hydrogel dressings offer numerous benefits with enhanced loading capacity and a moist-rich environment. However, their development is still limited by the accessibility of a suitable driven source outside the clinical environment for precise control over transdermal delivery kinetics. Here, we prepare a sulfonated poly(3,4-ethylenedioxythiophene) (PEDOT) polyelectrolyte hydrogel drug reservoir that responds to different stimuli-both endogenous cue (body temperature) and exogenous cue (electrical stimulation), for wearable on-demand transdermal delivery with enhanced efficacy. Functioned as both the drug reservoir and cathode in a Zn battery-powered iontophoresis patch, this dual-responsive hydrogel achieves high drug release efficiency (68.4 %) at 37 °C. Evaluation in hairless mouse skin demonstrates the efficacy of this technology by facilitating transdermal transport of 12.2 μg cm-2 dexamethasone phosphate when discharged with a 103 Ω external resistor for 3 h. The Zn battery-driven iontophoresis results in an effective treatment of atopic dermatitis, displaying reductions in epidermal thickness, mast cell infiltration inhibition, and a decrease in IgE levels. This work provides a new treatment modality for chronic epidermal diseases that require precise drug delivery in a non-invasive way.

Conductive hydrogel is considered to be one of the most potential sensing materials for wearable strain sensors. However, both the hydrophilicity of polymer chains and high water content severely inhibit the potential applications of hydrogel-based sensors in extreme conditions. In this study, a multicross-linked hydrogel was prepared by simultaneously introducing a double-network matrix, multiple conductive fillers, and free-moving ions, which can withstand an ultralow temperature below -80 °C. A superhydrophobic Ecoflex layer with a water contact angle of 159.1° was coated on the hydrogel using simple spraying and laser engraving methods. Additionally, the smart glove integrating five hydrogel strain sensors with a microprocessor was developed to recognize 12 types of diving gestures and synchronously transmit recognition results to smartphones. The superhydrophobic and antifreezing hydrogel strain sensor proposed in this study emerges promising potentials in wearable electronics, human-machine interfaces, and underwater applications.

Peripheral neural interfaces facilitate bidirectional communication between the nervous system and external devices, enabling precise control for prosthetic limbs, sensory feedback systems, and therapeutic interventions in the field of Bioelectronic Medicine. Intraneural interfaces hold great promise since they ensure high selectivity in communicating only with the desired nerve fascicles. Despite significant advancements, challenges such as chronic immune response, signal degradation over time, and lack of long-term biocompatibility remain critical considerations in the development of such devices. Here we report on the development and benchtop characterization of a novel design of an intraneural interface based on carbon fiber bundles. Carbon fibers possess low impedance, enabling enhanced signal detection and stimulation efficacy compared to traditional metal electrodes. We provided a 3D-stabilizing structure for the carbon fiber bundles made of PEDOT:PSS hydrogel, to enhance the biocompatibility between the carbon fibers and the nervous tissue. We further coated the overall bundles with a thin layer of elastomeric material to provide electrical insulation. Taken together, our results demonstrated that our electrode possesses adequate structural and electrochemical properties to ensure proper stimulation and recording of peripheral nerve fibers and a biocompatible interface with the nervous tissue.

Flexible conductive hydrogels have revolutionized the lives and are widely applied in health monitoring and wearable electronics as a new generation of sensing materials. However, the inherent low mechanical strength, sensitivity, and lack of rapid self-healing capacity results in their short life, poor detection accuracy, and environmental pollution. Inspired by the molecular structure of bone and its chemical characteristics, a novel fully physically cross-linked conductive hydrogel is fabricated by the introduction of nanohydroxyapatite (HAp) as the dynamic junction points. In detail, the dynamically cross-linked network, including multiple physical interactions, provides it with rapid self-healing ability and excellent mechanical properties (elongation at break (>1200%), tensile strength (174kPa), and resilience (92.61%)). Besides, the ions (Cl-, Li+, Ca2+) that move freely within the system impart outstanding electrical conductivity (2.46 ± 0.15 S m-1), high sensitivity (gauge factor, GF>8), good antifreeze (-40.2 °C), and humidity properties. The assembled sensor can be employed to sensitively detect various large human motions and subtle changes in behavior (facial expressions, speech recognition). Meanwhile, the hydrogel sensor can also degrade in phosphate-buffered saline solution without causing any environmental pollution. Therefore, the designed hydrogels may become a promising candidate material in the future potential applications for smart wearable sensors and electronic skin.

Conductive hydrogels have been widely applied in human-computer interaction, tactile sensing, and sustainable green energy harvesting. Herein, a double cross-linked network composite hydrogel (MWCNTs/CNWs/PAM/SA) by constructing dual enhancers acting together with PAM/SA was constructed. By systematically optimizing the compositions, the hydrogel displayed features advantages of good mechanical adaptability, high conductivity sensitivity (GF = 5.65, 53 ms), low hysteresis (<11 %), and shape memory of water molecules and temperature. The nanocellulose crystals (CNWs) were bent and entangled with the backbone of the polyacrylamide/ sodium alginate (PAM/SA) hydrogel network, which effectively transferred the external mechanical forces to the entire physical and chemical cross-linking domains. Multi-walled carbon nanotubes (MWCNTs) were filled into the cross-linking network of the hydrogel to enhance the conductivity of the hydrogel effectively. Notably, hydrogels are designed as flexible tactile sensors that can accurately recognize and monitor electrical signals from different gesture movements and temperature changes. It was also assembled as a friction nanogenerator (TENG) that continuously generates a stable open circuit voltage (28 V) for self-powered small electronic devices. This research provides a new prospect for designing nanocellulose and MWCNTs reinforced conductive hydrogels via a facile method.

The low electrical conductivity of conductive hydrogels limits their applications as soft conductors in bioelectronics. This low conductivity originates from the high water content of hydrogels, which impedes facile carrier transport between conductive fillers. This study presents a highly conductive and stretchable hydrogel nanocomposite comprising whiskered gold nanosheets. A dry network of whiskered gold nanosheets is fabricated and then incorporated into the wet hydrogel matrices. The whiskered gold nanosheets preserve their tight interconnection in hydrogels despite the high water content, providing a high-quality percolation network even under stretched states. Regardless of the type of hydrogel matrix, the gold-hydrogel nanocomposites exhibit a conductivity of ≈520 S cm-1 and a stretchability of ≈300% without requiring a dehydration process. The conductivity reaches a maximum of ≈3304 S cm-1 when the density of the dry gold network is controlled. A gold-adhesive hydrogel nanocomposite, which can achieve conformal adhesion to moving organ surfaces, is fabricated for bioelectronics demonstrations. The adhesive hydrogel electrode outperforms elastomer-based electrodes in in vivo epicardial electrogram recording, epicardial pacing, and sciatic nerve stimulation.

Ischemia/reperfusion (I/R) injury following myocardial infarction is a major cause of cardiomyocyte death and impaired cardiac function. Although clinical data show that metformin is effective in repairing cardiac I/R injury, its efficacy is hindered by non-specific targeting during administration, a short half-life, frequent dosing, and potential adverse effects on the liver and kidneys. In recent years, injectable hydrogels have shown substantial potential in overcoming drug delivery challenges and treating myocardial infarction. To this end, we developed a natural polymer hydrogel system comprising methacryloylated chitosan and methacryloylated gelatin modified with polyaniline conductive derivatives. In vitro studies demonstrated that the optimized hydrogel exhibited excellent injectability, biocompatibility, biodegradability, suitable mechanical properties, and electrical conductivity. Incorporating metformin into this hydrogel significantly extended the administration cycle, mitigated mitochondrial damage, decreased abnormal ROS production, and enhanced cardiomyocyte function. Animal experiments indicated that the metformin/hydrogel system reduced arrhythmia incidence, infarct size, and improved cardiac mitochondrial and overall cardiac function, promoting myocardial repair in I/R injury. Overall, the metformin-loaded conductive hydrogel system effectively mitigates mitochondrial oxidative damage and improves cardiomyocyte function, thereby offering a theoretical foundation for the potential application of metformin in cardioprotection.