Conductive Hydrogels Research Articles

Superhydrophobic, Anti-Freezing and Multi-Cross-Linked Wearable Hydrogel Strain Sensor for Underwater Gesture Recognition.

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.

Strong and tough anisotropic short-chain chitosan-based hydrogels with optimized sensing properties for flexible strain sensors

Conductive hydrogels are ideal candidates for developing flexible electronic devices, but they still cannot exhibit excellent strength, satisfactory toughness and high conductivity in sync, greatly limiting their further applications. Inspired by the structure-enhanced properties of natural tissues, we adopted a straightforward and efficient methodology for constructing strong and tough anisotropic short-chain chitosan-based hydrogels with salting-assisted tensile remodeling treatment. The anisotropic hydrogels present anisotropic mechanical and electrochemical performance due to the oriented arrangement of chitosan and P(AM-AA) macromolecular networks. The remarkable tensile strength, toughness, and conductivity of parallel-oriented hydrogels are up to 9.01 MPa, 32.77 MJ/m3, and 692.30 mS/m, respectively, which are much higher than that of isotropic and vertical-oriented hydrogels, verifying the structure-optimized mechanical and sensing performance. The anisotropic conductive polypolysaccharide hydrogels are assembled as strain sensors for real-time human movement monitoring, Morse code encryption and decryption transmission, and gesture prediction combined with a machine learning algorithm, providing new inspiration for blossoming strong, flexible electronic products.

Introductory Review of Soft Implantable Bioelectronics Using Conductive and Functional Hydrogels and Hydrogel Nanocomposites.

Interfaces between implantable bioelectrodes and tissues provide critical insights into the biological and pathological conditions of targeted organs, aiding diagnosis and treatment. While conventional bioelectronics, made from rigid materials like metals and silicon, have been essential for recording signals and delivering electric stimulation, they face limitations due to the mechanical mismatch between rigid devices and soft tissues. Recently, focus has shifted toward soft conductive materials, such as conductive hydrogels and hydrogel nanocomposites, known for their tissue-like softness, biocompatibility, and potential for functionalization. This review introduces these materials and provides an overview of recent advances in soft hydrogel nanocomposites for implantable electronics. It covers material strategies for conductive hydrogels, including both intrinsically conductive hydrogels and hydrogel nanocomposites, and explores key functionalization techniques like biodegradation, bioadhesiveness, injectability, and self-healing. Practical applications of these materials in implantable electronics are also highlighted, showcasing their effectiveness in real-world scenarios. Finally, we discuss emerging technologies and future needs for chronically implantable bioelectronics, offering insights into the evolving landscape of this field.

Mechanically robust and highly conductive bacterial cellulose hydrogels through synergy of directional freeze–thawing and salting-out for wearable sensors

It is urgent to develop high-performance conductive hydrogels that simultaneously exhibit high biocompatibility, mechanical robustness, exceptional conductivity and frost resistance to fulfil the requirements of wearable flexible sensors. Herein, we present a simple and integrated approach for designing iso/anisotropic bacterial cellulose (BC) hydrogels by immersing the as-prepared polyvinyl alcohol (PVA)–BC–Borax hydrogels in saturated NaCl solutions using a salting-out effect to assist the non–/directional freeze–thawing strategy. Benefitting from the synergistic strengthening of molecular interactions, including hydrogen, coordination, and boron ester bonds, as well as the enhanced PVA and BC crystallinity resulting from the salting-out effect, the tensile strength (0.8–3.2 MPa) and high ionic conductivity (61.5–136.2 mS/cm) of isotropic hydrogels (PVA–BC–Borax/NaCl) can be well tuned by adjusting the feeding mass fractions of PVA, borax and BC. The optimised hydrogel, PVA7.5%–BC0.45%–Borax0.375%/NaCl, demonstrated remarkable mechanical properties (3.2 MPa, 295.1 %), ionic conductivity (72.6 mS/cm) and good anti-freezing properties (–40.8 °C), maintaining excellent conductivity (61.8 mS/cm) even at –20 °C due to the introduction of NaCl. When subjected to directional freeze–thawing cycles, the D(Directional)-PVA7.5%–BC0.45%–Borax0.375%/NaCl hydrogel, with its organised layers and larger pore–sized structures, exhibited higher breaking elongation (609.2 %) and ionic conductivity (81.6 mS/cm) than its isotropic counterpart (295.1 %, 72.6 mS/cm). The D-PVA7.5%–BC0.45%–Borax0.375%/NaCl hydrogel was successfully used as a strain sensor for detecting a variety of human movements, showing excellent responsiveness to external stimuli, thereby demonstrating its potential applications in human–machine interaction, flexible sensing and bioelectronics.

Attapulgite-Reinforced Cellulose Hydrogels with High Conductivity and Antifreezing Property for Flexible Sensors.

Ionic conductive cellulose hydrogels are some of the most promising candidates for flexible sensors. However, it is difficult to simultaneously prepare cellulose hydrogels with high mechanical strength, good ionic conductivity, and antifreeze performance. In this work, a natural clay (attapulgite)-reinforced cellulose hydrogel was fabricated. Through a one-pot method, cellulose and attapulgite were dispersed in a concentrated ZnCl2 solution. The obtained hydrogel exhibited a dual network of hydrogen bonds and Zn2+-induced ionic interactions. Attapulgite serves as an inorganic filler that can regulate the hydrogen-bonding density among cellulose molecules and provides abundant channels for fast ion transport. By optimizing the attapulgite loading, a mechanically strong (compressive strength up to 1.10 MPa), tough (fracture energy up to 0.36 MJ m-3), highly ionic conductive (4.15 S m-1), and freezing-tolerant hydrogel was prepared. These hydrogels can be used for sensitive and stable human motion sensing, demonstrating their great potential for healthcare applications.

Phytic acid-based super antifreeze multifunctional conductive hydrogel for human motion monitoring and energy harvesting devices

Conductive hydrogels have broad application prospects in the field of self-powered sensors and energy harvesting devices due to their good electrical conductivity and flexibility. However, at low temperatures, conductive hydrogels are usually frozen, resulting in problems such as poor electrical conductivity and flexibility, which seriously hinder the application of these fields. To address these challenges, phytic acid (PA) was employed as the crosslinker and antifreezing agent in this study. Polyvinyl alcohol (PVA), 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPS), chitosan (CS), and PA were used as raw materials to successfully synthesize PVA/AMPS/CS/PA (PACP) multifunctional conductive hydrogels with outstanding antifreeze and water retention properties (freezing point below −80 °C, 30-day water loss rate of 3.5%). In addition, PACP hydrogels exhibit exceptional electrical conductivity of up to 9.4 S/m, along with antibacterial and biocompatible properties, enabling their utilization as wearable sensors on human skin tissue. Notably, the PACP hydrogel-based triboelectric nanogenerator (PACP-TENG) excels in accurately monitoring human motion and powering small electronic devices, facilitating remote control of small light switches. The resulting open circuit voltage is as high as 314 V at 25 °C and about 110 V at low temperature. Therefore, PACP hydrogels with excellent properties are expected to expand their applications in these fields.

Tannic Acid-Enabled Antioxidant and Stretchable MXene/Silk Strain Sensors for Diving Training Healthcare.

MXene-based conductive hydrogels hold significant promise as epidermal sensors, yet their susceptibility to oxidation represents a formidable limitation. This study addresses this challenge by incorporating MXene into a tannic acid (TA) cross-linked silk fibroin matrix. The resulting conductive hydrogel (denoted as e-dive) exhibits favorable characteristics such as adjustable mechanical properties, self-healing capabilities (both mechanically and electrically), and strong underwater adhesion. The existence of a percolation network of MXene within the nanocomposites guarantees good electrical conductivity. Importantly, the surface interaction of MXene nanosheets with the hydrophobic moiety from TA substantially reduced moisture and oxygen interactions with MXene, thereby effectively mitigating MXene oxidation within hydrogel matrices. This preservation of the electrical characteristics ensures prolonged functional stability. Furthermore, the e-dive demonstrates inherent antibacterial properties, making it suitable for use in underwater environments where bacterial contamination is a concern. The utilization of this advanced e-dive system extends to the correction of diving postures and the facilitation of underwater healthcare and security alerts. Our study presents a robust methodology for enhancing the stability of MXene-based conductive hydrogel electronics, thereby expanding their scope of potential applications.

Programming Hydrogen Bonds for Reversible Elastic-Plastic Phase Transition in a Conductive Stretchable Hydrogel Actuator with Rapid Ultra-High-Density Energy Conversion and Multiple Sensory Properties.

Smart hydrogels have recently garnered significant attention in the fields of actuators, human-machine interaction, and soft robotics. However, when constructing large-scale actuated systems, they usually exhibit limited actuation forces (≈2kPa) and actuation speeds. Drawing inspiration from hairspring energy conversion mechanism, an elasticity-plasticity-controllable composite hydrogel (PCTA) with robust contraction capabilities is developed. By precisely manipulating intermolecular and intramolecular hydrogen-bonding interactions, the material's elasticity and plasticity can be programmed to facilitate efficient energy storage and release. The proposed mechanism enables rapid generation of high contraction forces (900kPa) at ultra-high working densities (0.96MJm-3). Molecular dynamics simulations reveal that modifications in the number and nature of hydrogen bonds lead to a distinct elastic-plastic transition in hydrogels. Furthermore, the conductive PCTA hydrogel exhibits multimodal sensing capabilities including stretchable strain sensing with a wide sensing range (1-200%), fast response time (180ms), and excellent linearity of the output signal. Moreover, it demonstrates exceptional temperature and humidity sensing capabilities with high detection accuracy. The strong actuation power and real-time sensory feedback from the composite hydrogels are expected to inspire novel flexible driving materials and intelligent sensing systems.

Preparation of accelerated-wound-healing lignin/dopamine-based nano-Fe3O4 hydrogels in sensing

Flexible conductive hydrogels hold great promise for applications in motion and medical detection. It is difficult to produce conductive hydrogel epidermal sensors in wearable hydrogels with dependable adhesion, sensing, and wound-healing properties. Nano-Fe3O4 was used as physical cross-linking points in the polyacrylamide/polyvinyl alcohol double network (PP) to increase the strain capacity of the hydrogel. The conductive lignin-dopamine (LD) was immobilized on the surface of Fe3O4 particles, and the LD-coated Fe3O4 was then incorporated into the double network hydrogel to create the PP/LD/Fe3O4 hydrogel. This work was done to look into the possibility of using Fe3O4 hydrogels as flexible strain sensors. The addition of LD/Fe3O4 caused the composite hydrogel to strain up to 124 %, with a modulus of elasticity of 21,308 Pa and electrical conductivity as high as 2.3 S•m−1 following the introduction of LD/Fe3O4. Moreover, the PP/LD/Fe3O4 hydrogel's adhesive qualities offered adequate antimicrobial properties and promoted wound healing. These results indicate that the developed electricity-responsive and tissue-adhesive hydrogel dressing offers a candidate to serve as a tissue sealant for wound healing.

Preparation and motion-sensing properties of ion/electron mixed conductive hydrogels fabricated by carbon-coated sepiolite nanofibers

Hydrogels have experienced significant advancements owing to their versatile applications in biomedicine, wound care, food packaging, and smart devices. The pursuit of environmentally sustainable and scalable hydrogel production methods remains a primary research objective. This study introduces an innovative hydrogel fabrication technique involving the integration of surface-modified sepiolite nanofibers with polyacrylamide (PAM), resulting in the formation of sepiolite-based composite hydrogels (PASSC). These hydrogels exhibit both ionic and electronic conductivity, along with improved mechanical properties and rheological behavior. PASSC hydrogels demonstrate remarkable fatigue resistance, maintaining mechanical integrity over 10,000 stress cycles, thereby indicating their potential for long-term applications. Additionally, these hydrogels exhibit distinctive mixed conductivity, which enhances their strain sensitivity and efficacy in strain sensing. The ability of PASSC hydrogels to accurately detect a range of movements underscores their versatility and reliability in monitoring strain changes across diverse applications.

Multifunctional Nano‐Conductive Hydrogels With High Mechanical Strength, Toughness and Fatigue Resistance as Self‐Powered Wearable Sensors and Deep Learning‐Assisted Recognition System

AbstractHigh mechanical strength, toughness, and fatigue resistance are essential to improve the reliability of conductive hydrogels for self‐powered sensing. However, achieving mutually exclusive properties simultaneously remains challenging. Hence, a novel directed interlocking strategy based on topological network structure and mechanical training is proposed to construct tough hydrogels by optimizing the network structure and modulating the orientation of molecular chains. Combining Zn2+ crosslinked cellulose nanofibers (CNFs) and a polyacrylamide‐poly(vinyl alcohol) double‐network, the unique interlocked‐network structure exhibits an enhanced toughening effect due to hydrogen bonding and metal‐ligand interactions. The aligned nanocrystalline domains achieved by training further contribute to an increase in the toughness and fatigue thresholds. This innovative approach synergistically enhances the mechanical properties of the nano‐conductive hydrogel, achieving a maximum tensile strength of 4.98 MPa and a toughness of 48 MJ m−3. Notably, the CNFs template with anchored polyaniline, when oriented through mechanical training, forms a unique directional conductive pathway, which significantly enhances the power output performance. Besides, a motion recognition system based on a self‐powered sensing device is designed with the assistance of deep learning techniques to accurately identify human motion behaviors. This work showcases a potentially transformative flexible electronic material for self‐powered sensing systems and intelligent recognition systems.

Conductive, injectable, and self-healing collagen-hyaluronic acid hydrogels loaded with bacterial cellulose and gold nanoparticles for heart tissue engineering

The increasing demand for advanced biomaterials in nerve tissue engineering presents numerous challenges due to the complexity of nerve tissues and the need for materials that can accurately replicate their intricate structure and function. In response, this study introduces a novel injectable hydrogel that is thermosensitive, self-healing, and conductive, offering promising potential for heart and nerve tissue engineering applications. The hydrogel is based on collagen and hyaluronic acid functionalized with 3-aminopropyl-triethoxysilane (APTES)-grafted oxidized bacterial cellulose and gold nanoparticles (~50 nm). Rheological analysis reveals a substantial enhancement in the elastic modulus of the collagen-hyaluronic acid matrix with the incorporation of bacterial cellulose/gold nanoparticles, improving by an order of magnitude at 1 % strain. This improvement comes with a slight decrease in gelation temperature, from 36 °C to 32 °C. Besides thermo-sensitivity, the nanocomposite hydrogel exhibits a remarkable self-sealing response (about 80 % effectiveness) due to reversible physical crosslinking. Electrical spatial resistance measurements on human embryonic stem cell-derived cardiomyocytes-loaded hydrogels yield a value of ~0.1 S/m, which is suitable for electrical stimulation. In vitro extracellular field potential measurements also affirm the hydrogel's potential as an injectable scaffold for heart tissue engineering, i.e., the electrically stimulated human stem cells exhibit 47 beats per minute with a cell discharge (depletion) of 5.47 μv. A rapid gel formation in the physiological temperature (about 2 min) and high H9C2 cytotoxicity (viability of >90 % after 72 h incubation) is attainable. The developed collagen-based nanocomposite hydrogel offers an injectable, thermosensitive, and self-healing biomaterial platform for nerve or myocardium regeneration.

PNIPAAm-based temperature responsive ionic conductive hydrogels for flexible strain and temperature sensing

Conductive hydrogels have received much attention in the field of flexible wearable sensors due to their outstanding flexibility, conductivity, sensitivity and excellent compatibility. However, most conductive hydrogels mainly focus on strain sensors to detect human motion and lack other features such as temperature response. Herein, we prepared a strain and temperature dual responsive ionic conductive hydrogel (PPPNV) with an interpenetrating network structure by introducing a covalent crosslinked network of N-isopropylacrylamide (NIPAAm) and 1-vinyl-3-butylimidazolium bromide (VBIMBr) into the skeleton of the hydrogel composed of polyvinylalcohol (PVA) and polyvinylpyrrolidone (PVP). The PPPNV hydrogel exhibited excellent anti-freezing properties (−37.34 °C) and water retention with high stretchability (∼930 %) and excellent adhesion. As a wearable strain sensor, the PPPNV hydrogel has good responsiveness and stability to a wide range of deformations and exhibits high strain sensitivity (GF=2.6) as well as fast response time. It can detect large and subtle body movements with good signal stability. As wearable temperature sensors, PPPNV hydrogels can detect human physiological signals and respond to temperature changes, and the volumetric phase transition temperature (VPTT) can be easily controlled by adjusting the molar ratio of NIPAAm to VBIMBr. In addition, a bilayer temperature-sensitive hydrogel was prepared with the temperature responsive hydrogel by two-step synthesis, which shows great promising applications in temperature actuators.

Molecular Bridging Induced Anti-salting-out Effect Enabling High Ionic Conductive ZnSO4-based Hydrogel for Quasi-solid-state Zinc Ion Batteries.

Hydrogel electrolytes (HEs) hold great promise in tackling severe issues emerging in aqueous zinc-ion batteries, but the prevalent salting-out effect of kosmotropic salt causes low ionic conductivity and electrochemical instability. Herein, a subtle molecular bridging strategy is proposed to enhance the compatibility between PVA and ZnSO4 from the perspective of hydrogen-bonding microenvironment re-construction. By introducing urea containing both an H-bond acceptor and donor, the broken H-bonds between PVA and H2O, initiated by the SO42--driven H2O polarization, could be re-united via intense intermolecular hydrogen bonds, thus leading to greatly increased carrying capacity of ZnSO4. The urea-modified PVA-ZnSO4 HEs featuring a high ionic conductivity up to 31.2 mS cm-1 successfully solves the sluggish ionic transport dilemma at the solid-solid interface. Moreover, an organic solid-electrolyte-interphase can be derived from the in-situ electro-polymerization of urea to prohibit H2O-involved side reactions, thereby prominently improving the reversibility of Zn chemistry. Consequently, Zn anodes witness an impressive lifespan extension from 50 h to 2200 h at 0.1 mA cm-2 while the Zn-I2 full battery maintains a remarkable Coulombic efficiency (>99.7%) even after 8000 cycles. The anti-salting-out strategy proposed in this work provides an insightful concept for addressing the phase separation issue of functional HEs.

Polymeric silk fibroin hydrogel as a conductive and multifunctional adhesive for durable skin and epidermal electronics.

Silk fibroin (SF)-based hydrogels are promising multifunctional adhesive candidates for real-world applications in tissue engineering, implantable bioelectronics, artificial muscles, and artificial skin. However, developing conductive SF-based hydrogels that are suitable for the micro-physiological environment and maintain their physical and chemical properties over long periods of use remains challenging. Herein, we developed an ion-conductive SF hydrogel composed of glycidyl methacrylate silk fibroin (SilMA) and bioionic liquid choline acylate (ChoA) polymer chains, together with the modification of acrylated thymine (ThyA) and adenine (AdeA) functional groups. The resulting polymeric ion-conductive SF composite hydrogel demonstrated high bioactivity, strong adhesion strength, good mechanical compliance, and stretchability. The formed hydrogel network of ChoA chains can coordinate with the ionic strength in the micro-physiological environment while maintaining the adaptive coefficient of expansion and stable mechanical properties. These features help to form a stable ion-conducting channel for the hydrogel. Additionally, the hydrogel network modified with AdeA and ThyA, can provide a strong adhesion to the surface of a variety of substrates, including wet tissue through abundant hydrogen bonding. The biocompatible and ionic conductive SF composite hydrogels can be easily prepared and incorporated into flexible skin or epidermal sensing devices. Therefore, our polymeric SF-based hydrogel has great potential and wide application to be an important component of many flexible electronic devices for personalized healthcare.

Synthesis of Self‐Adhesive, Self‐Healing and Antifreeze Conductive Hydrogels for Flexible Strain sensors

Abstract Recently, significant progress has been made regarding conductive hydrogels‐based flexible sensors in health detection, electronic skin, soft robots, etc. However, the requirement of bonding with the substrate through the adhesive tape, brokenness sensitivity, and degradation of performance under low‐temperature environments, strongly limit the wide applications of conductive hydrogels in flexible sensors. To solve these problems, this study introduces lithium chloride (LiCl) into poly(vinyl alcohol)/tannic acid/polyacrylamide (PVA/TA/PAM) hydrogels to endow the hydrogels with excellent conductivity and antifreeze properties. In addition, the addition of tannic acid (TA) and zwitterionic 3‐[Dimethyl‐[2‐(2‐methylprop‐2‐enoyloxy)ethyl]azaniumyl]propane‐1‐sulfonate (SBMA) enables the hydrogel to have good self‐healing performance (after 72 h of healing at 20 °C, the healing efficiency of fracture stress is 24%, and the healing efficiency of fracture strain is 52%) and adhesion (the adhesion strength to paper at 20 °C is 14.12 KPa). The sensors based on PVA/TA/PAM composite hydrogels exhibit good sensibility, stability, and durability, and can respond quickly to human joint activities (finger bending, wrist bending, arm bending, and leg bending). Therefore, the multifunctional PVA/TA/PAM composite hydrogel demonstrates significant potential for applications in flexible strain sensors under extreme environments.

Flexible and antibacterial conductive hydrogels based on silk fibroin/polyaniline/AgNPs for motion sensing and wound healing promotion under electrical stimulation.

Flexible conductive hydrogel-based electronic skin (E-skin) for simultaneous biotherapeutics and sensing applications is one of the current research directions. In this study, conductive and homogeneous silk fibroin/polyaniline/AgNP complexes (SPAg complexes) were prepared with the assistance of silk fibroin, which greatly optimized the compatibility of PANI with the hydrogel matrix. Then, SPAg was introduced into the covalently crosslinked polymer network to prepare poly(acrylamide-co-sulfobetaine methacrylate) - SPAg hydrogels (labeled as PSPAg hydrogels). The PSPAg hydrogels exhibit good biocompatibility, excellent mechanical properties, superb adhesive performance, and fantastic sensing capabilities. Being connected to a smartphone via a Bluetooth system, the SPAg hydrogel-based E-skin was employed to accurately monitor human movements including vigorous joint movements and subtle facial micro-expressions. Finally, benefiting from the synergistic effect of antimicrobial and exogenous electrical stimulation, through promoting angiogenesis and accelerating collagen production in diabetic wounds, PSPAg E-skin successfully facilitates rapid diabetic wound healing. Therefore, the multifunctional PSPAg hydrogel-based E-skin shows great promise for applications in wearable devices and bioelectronics.

Versatile conductive hydrogel orchestrating neuro–immune microenvironment for rapid diabetic wound healing through peripheral nerve regeneration

Diabetic wound (DW), notorious for prolonged healing processes due to the unregulated immune response, neuropathy, and persistent infection, poses a significant challenge to clinical management. Current strategies for treating DW primarily focus on alleviating the inflammatory milieu or promoting angiogenesis, while limited attention has been given to modulating the neuro-immune microenvironment. Thus, we present an electrically conductive hydrogel dressing and identify its neurogenesis influence in a nerve injury animal model initially by encouraging the proliferation and migration of Schwann cells. Further, endowed with the synergizing effect of near-infrared responsive release of curcumin and nature-inspired artificial heterogeneous melanin nanoparticles, it can harmonize the immune microenvironment by restoring the macrophage phenotype and scavenging excessive reactive oxygen species. This in-situ formed hydrogel also exhibits mild photothermal therapy antibacterial efficacy. In the infected DW model, this hydrogel effectively supports nerve regeneration and mitigates the immune microenvironment, thereby expediting the healing progress. The versatile hydrogel exhibits significant therapeutic potential for application in DW healing through fine-tuning the neuro-immune microenvironment.

Dual design strategy for carboxymethyl cellulose-polyaniline composite hydrogels as super-sensitive amphibious sensors

Conductive hydrogels as ideal candidate materials for flexible sensors have exhibited many promising applications. However, complex application environments, such as low temperatures or underwater conditions, have introduced new requirements for hydrogel sensors. Herein, a high-performance conductive hydrogel based on carboxymethyl cellulose-polyaniline (CMC-PANI) submicron spheres, poly (vinyl alcohol) (PVA) and phytic acid (PA) was designed and fabricated via a dual design strategy. CMC-PANI particles were introduced to not only empower the good electromechanical performance to the hydrogels, but also enhance the mechanical properties. The obtained hydrogel exhibited good mechanical property, anti-freezing, anti-swellable behavior and recyclable performance. Resistive-type strain sensors assembled by the prepared hydrogels exhibited high pressure sensitivity (34.17×10−2 kPa−1) and fast response time (100 ms), which can clearly detect the pulse beats. Moreover, the hydrogel sensors can achieve long-term stability, high sensitivity and fatigue resistance as an underwater sensor. Based on these favorable performances, the conductive polymer hydrogels may open up an enticing avenue for functional soft materials in health diagnostic and electronic components.

Highly-stable, injectable, conductive hydrogel for chronic neuromodulation

Electroceuticals, through the selective modulation of peripheral nerves near target organs, are promising for treating refractory diseases. However, the small sizes and the delicate nature of these nerves present challenges in simplifying the fixation and stabilizing the electrical-coupling interface for neural electrodes. Herein, we construct a robust neural interface for fine peripheral nerves using an injectable bio-adhesive hydrogel bioelectronics. By incorporating a multifunctional molecular regulator during network formation, we optimize the injectability and conductivity of the hydrogel through fine-tuning reaction kinetics and multi-scale interactions within the conductive network. Meanwhile, the mechanical and electrical stability of the hydrogel is achieved without compromising its injectability. Minimal tissue damage along with low and stable impedance of the injectable neural interface enables chronic vagus neuromodulation for myocardial infarction therapy in the male rat model. Our highly-stable, injectable, conductive hydrogel bioelectronics are readily available to target challenging anatomical locations, paving the way for future precision bioelectronic medicine.