Ion Gel Research Articles

Cellulose nanocomposite tough hydrogels: synergistic self‐healing, adhesive and strain‐sensitive properties

AbstractRecent advancements are notable in electrically conductive hydrogels emulating human skin functions. However, a significant challenge remains: crafting a single conductive gel that integrates self‐healing, robust mechanical strength, and excellent electrical traits. Our innovation lies in a strong, lightweight, curable gel achieved through multiple coordination bonds between cellulose crystals and acid‐treated multi‐walled carbon nanotubes (MWCNTs) in a polymer network. Embedded MWCNTs act as dynamic bridges within a porous structure, giving exceptional mechanical performance. Reversible coordination interactions confer remarkable recovery and reliable mechanical and electrical self‐healing. Additionally, these ionic gels function as adaptable stress sensors, detecting significant movements like finger and joint motions. This work introduces MWCNT‐incorporated nanomaterials with good stretchability, high ion conductivity, remarkable self‐healing nature, and good stress sensitivity. Such proteins hold promise for electronic sensors, wearable devices, and healthcare monitoring, unveiling a path to diverse applications. Our study addresses challenges and unlocks possibilities for materials that can adapt, withstand, and sense in innovative ways. © 2024 Society of Chemical Industry.

Supramolecular Ionic Liquid Gels with Tunable Conductivity Based on Host–Guest Interaction

Supramolecular Ionic Liquid Gels with Tunable Conductivity Based on Host–Guest Interaction

Flexible Iontronic Tactile Sensors Based on Silver Nanowire Electrode with Sandpaper-Roughened Surface and Ionic Liquid Gel Electrolyte with Porous Foam Structure for Wearable Sensing Applications

Flexible Iontronic Tactile Sensors Based on Silver Nanowire Electrode with Sandpaper-Roughened Surface and Ionic Liquid Gel Electrolyte with Porous Foam Structure for Wearable Sensing Applications

Reusable, Green, Portable Ionogels Based on Terpyridine-Imidazole Salt for Visual Monitoring of Pork Spoilage.

Ionogels have emerged as a promising approach because they combine the advantageous properties of ionic liquids and gels. Herein, a novel gelator bearing terpyridine and imidazolium salt units was designed and synthesized, which assembled into ionogels in three ionic liquids by a heating-cooling procedure. The properties of ionogels were characterized by FT-IR, UV-vis spectroscopy, POM, XRD, and rheology, and resonance light scattering and opacity measurements were conducted to investigate the gelation kinetics. Furthermore, the ionogels incorporating pH-sensitive dyes (BTB and MR) were exploited as colorimetric sensor to monitor total volatile basic nitrogen (TVB-N) of meat at -4 °C, which can easily and reliably estimate the quality of meat by naked eye recognition, and the results demonstrated a positive correlation between the color variation and TVB-N levels. Notably, the hydrophobic ionogel indicators are more suitable for potential application at high humidity thanks to their antiswelling advantage, which could prevent the inaccurate information produced by hydrogel indicators. In addition, the ionogels could be reused up to three times as colorimetric indicators, suggesting potential applications and competitiveness. Our research sheds new light on the novel application of ionogels in the food industry.

Influence of Carboxymethyl Cellulose as a Thickening Agent for Glauber's Salt-Based Low Temperature PCM.

This work is focused on a novel, promising low temperature phase change material (PCM), based on the eutectic Glauber's salt composition. To allow phase transition within the refrigeration range of temperatures of +5 °C to +12 °C, combined with a high repeatability of melting-freezing processes, and minimized subcooling, the application of three variants of sodium carboxymethyl cellulose (Na-CMC) with distinct molecular weights (700,000, 250,000, and 90,000) is considered. The primary objective is to optimize the stabilization of this eutectic PCM formulation, while maintaining the desired enthalpy level. Preparation methods are refined to ensure repeatability in mixing components, thereby optimizing performance and stability. Additionally, the influence of Na-CMC molecular weight on stabilization is examined through differential scanning calorimetry (DSC), T-history, and rheology tests. The PCM formulation of interest builds upon prior research in which borax, ammonium chloride, and potassium chloride were used as additives to sodium sulfate decahydrate (Glauber's salt), prioritizing environmentally responsible materials. The results reveal that CMC with molecular weights of 250 kg/mol and 90 kg/mol effectively stabilize the PCM without phase separation issues, slowing crystallization kinetics. Conversely, CMC of 700 kg/mol proved ineffective due to the disruption of gel formation at its low gel point, hindering higher concentrations. Calculations of ionic concentration indicate higher Na ion content in PCM stabilized with 90 kg/mol CMC, suggesting increased ionic interactions and gel strength. A tradeoff is discovered between the faster crystallization in lower molecular weight CMC and the higher concentration required, which increases the amount of inert material that does not participate in the phase transition. After thermal cycling, the best formulation had a latent heat of 130 J/g with no supercooling, demonstrating excellent performance. This work advances PCM's reliability as a thermal energy storage solution for diverse applications and highlights the complex relationship between Na-CMC molecular weight and PCM stabilization.

Metal-Halogen Interactions Inducing Phase Separation for Self-Healing and Tough Ionogels with Tunable Thermoelectric Performance.

Ionic liquid-based thermoelectric gels become a compelling candidate for thermoelectric power generation and sensing due to their giant thermopower, good thermal stability, high flexibility, and low-cost production. However, the materials reported to date suffer from canonical trade-offs between self-healing ability, stretchability, strength, and ionic conductivity. Herein, a self-healing and tough ionogel (PEO/LiTFSI/EmimCl) with tunable thermoelectric properties by tailoring metal-halogen bonding interactions, is developed. Different affinities between polymer matrix and salts are exploited to induce phase separation, resulting in simultaneous enhancement of ionic conductivity and mechanical strength. Molecular dynamics (MD) simulations and spectroscopic analyses show that Cl- ions impair the lithium-ether oxygen coordination, leading to changes in chain conformation. The migration difference between cations and anions is thus widened and a transition from n-type to p-type thermoelectric ionogels is realized. Furthermore, the dynamic interactions of metal-ligand coordination and hydrogen bonding yield autonomously self-healing capability, large stretchability (2000%), and environment-friendly recyclability. Benefiting from these fascinating properties, the multifunctional PEO-based ionogels are applied in sensors, supercapacitors, and thermoelectric power generation modules. The strategy of tuning solvation dominance to address the trade-offs in thermoelectric ionogels and optimize their macroscopic properties offers new possibilities for the design of advanced ionogels.

Double-sided microstructured flexible iontronic pressure sensor with wide linear sensing range

Iontronic pressure sensors have garnered significant attention for their potential in wearable electronic devices. While simple microstructures can enhance sensor sensitivity, the majority of them predominantly amplify sensitivity at lower pressure ranges and fail to enhance sensitivity at higher pressure ranges, leading to nonlinearity. In the absence of linear sensitivity in a pressure sensor, users are unable to derive precise information from its output, necessitating further signal processing. Hence, crafting a linearity flexible pressure sensor through a straightforward approach remains a formidable task. Herein, a double-sided microstructured flexible iontronic pressure sensor is presented with wide linear sensing range. The ionic gel is made by 1-Ethyl-3-methylimidazolium bis(tri-fluoromethylsulfonyl)imide (EMIM:TFSI) into the matrix of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), which acts as active layer, featuring irregular microstructures (IMS) and pyramid microstructures (PMS) on both sides. Unlike previous complex methods, IMS and uniform PMS are easily and achieved through pattern transfer from a sandpaper mold and micro-pyramid template. The iontronic pressure sensor exhibits exceptional signal linearity with R2 values of 0.9975 and 0.9985, in the wide pressure range from 100 to 760 kPa and 760 kPa to 1000 kPa, respectively. This outstanding linearity and wide sensing range stem from a delicate balance between microstructure compression and mechanical alignment at the ionic gel interface. This study provides valuable insights into achieving linear responses by strategically designing microstructures in flexible pressure sensors, with potential applications in intelligent robots and health monitoring.

N-Type ion gel gated vertical organic electrochemical transistors based on benzodifurandione-based Oligo(p-phenylene vinylene)s

Organic electrochemical transistors (OECTs) using aqueous gate dielectrics have garnered significant interest for bioelectronic applications. However, their viability for long-term use in neuromorphic computing and synaptic devices is limited due to their short-term functionality. In this study, we synthesize two benzodifurandione-based oligo (p-phenylene vinylene) polymers, BDOPV-TCNVT and ClBDOPV-TCNVT, and investigate their electrochemical transistor properties using quasi-solid-state ion gel-gated vertical OECTs (v-OECTs). Compared to BDOPV-TCNVT, the chlorinated ClBDOPV-TCNVT demonstrates lower frontier molecular orbitals and easier electrochemical doping. The higher volumetric capacitance of as-spun ClBDOPV-TCNVT (1.94 F cm−3) compared to as-spun BDOPV-TCNVT films (1.49 F cm−3) is mainly attributed to the easier ion infiltration resulting from its lower crystallinity with mixed chain orientation. The quasi-solid-state v-OECTs based on both polymers (as-spun) exhibit transconductance (gm) of 0.06–0.08 mS. Following thermal treatments, the gm gradually decreases for both polymers due to enhanced edge-on ordering with tight interchain packing, hindering ion penetration. Despite the poor electrochemical doping by quasi-solid-state ion gel gated dielectrics, the enlarged area and decreased channel length in v-OECTs (compared to parallel OECTs) can enhance the gm. Further optimization of v-OECTs requires tailored material designs specifically suited for efficient vertical charge transport together with ion infiltration.

Eutectogels as Promising Materials in Biocatalysis

AbstractThe entrapment of deep eutectic solvents (DES) and eutectic systems into porous scaffolds renders a new class of soft and nonvolatile materials called eutectogels that have recently stepped into the spotlight in different areas ranging from electronics to drug delivery. Recent progress in the use of DES in biocatalysis, where they have been demonstrated to improve substrate supply, conversion, and enzyme stability, has opened an unparalleled opportunity to exploit the merits of eutectogels for immobilizing biological catalysts. The resulting functional materials could outperform traditional hydrogels and ionic liquid gels, offering fresh perspectives to broaden the application scope of many enzymes. In this perspective, we go into the potential of eutectogels as innovative scaffolds that support biocatalytic reactions and discuss different applications where these systems could show plain benefits compared to traditional materials. Future directions for this newly developed technology are highlighted.

Sulfonated Chitosan Gel Membrane with Confined Amine Carriers for Stable and Efficient Carbon Dioxide Capture.

Capturing carbon dioxide (CO2) from flue gases is a crucial step towards reducing CO2 emissions. Among the various carbon capture methods, facilitated transport membranes (FTMs) have emerged as a promising technology for CO2 capture owing to their high efficiency and low energy consumption in separating CO2. However, FTMs still face the challenge of losing mobile carriers due to weak interaction between the carriers and membrane matrix. Herein, we report a sulfonated chitosan (SCS) gel membrane with confined amine carriers for effective CO2 capture. In this structure, diethylenetriamine (DETA) as a CO2-mobile carrier is confined within the SCS gel membrane via electrostatic forces, which can react reversibly with CO2 and thus greatly facilitate its transport. The SCS ion gel membrane allows for the fast diffusion of amine carriers within it while blocking the diffusion of nonreactive gases, like N2. Thus, the prepared membrane exhibits exceptional CO2 separation capabilities when tested under simulated flue gas conditions with CO2 permeance of 1155 GPU and an ultra-high CO2/N2 selectivity of above 550. Moreover, the membrane retains a stable separation performance during the 170 h continuous test. The excellent CO2 separation performance demonstrates the high potential of gel membranes for CO2 capture from flue gas.

In Situ Study on the Structural Evolution of Flexible Ionic Gel Sensors

With the development of society, the demand for smart coatings is increasing. The development of flexible strain sensors using block copolymer self-assembled ionic gel materials provides a promising method for promoting the development of smart coatings. The ionic liquid in the ionic part of the material is crucial for the performance of the sensor. In this study, the structural changes within FDA/dEAN (self-assembly of acrylated Pluronic F127 (F127-DA) in partially deuterated ethylammonium nitrate (dEAN)) triblock copolymer ionic gel during uniaxial tensile flow were characterized using an in situ SAXS technique. The results revealed that the characteristics of the responses of the ionic gel to strain resistance were intricately linked to the evolution of its microstructure during the tensile process. At low levels of strain, the face-centered cubic lattice arrangement of the micelles tended to remain unchanged. However, when subjected to higher strains, the molecular chains aligned along the stretching direction, resulting in a more ordered structure with reduced entropy. This alignment led to significant disruption in bridging structures within the material. Furthermore, this research explored the impact of the stretching rate on the relaxation process. It was observed that higher stretching rates led to decreases in the average relaxation time, indicating rate dependence in the microstructure’s behavior. These findings provide valuable insights into the behavior and performance of flexible strain sensors based on ionic gel materials in smart coatings.

Preparation and drug release performance of different gelation type polysaccharide/β-lactoglobulin fiber composite gels

Self-assembled protein fibers have attracted much attention in the fields of medicine and food because of their high aspect ratio, polymorphic structure and strong surface hydrophobicity. In this study, three different gelation types of polysaccharides/β-lactoglobulin fiber (Fblg) composite gels, including ionic alginate-Fblg gels, synergistic xanthan-Fblg gels, and double network agar-Fblg gels, were first prepared. The interactions between the polysaccharides and the Fblgs, the microstructure and mechanical properties of the composite gels were investigated using the light scattering, scanning electron microscopy, rheology and texture analysis in order to reveal their formation mechanisms. Then the loading and release properties of the water-soluble drug 5-fluorouracil (5-FU) and the hydrophobic drug curcumin (Cur) through these composite gels were further studied with release mechanisms determined by fitting different release models. It was found that the mechanical properties of the composite gels were determined by the mesh density of the three-dimensional networks formed inside the gels. The network structure and mechanical strength of the alginate-Fblg gels became weaker with the increase of Fblg content at pH 4 due to their attractive interaction which hindered the binding of Ca2+ to ALG, while the network and the strength of the alginate-Fblg gels didn't change much at pH 7 due to the repulsion between Alg and Fblg. The xanthan-Fblg gels formed lamellar structures with enhanced gel network and mechanical strength due to the hydrogen bonding and the electrostatic interaction with Fblg. The Agar-Fblg composite gel formed at 60 °C (above the gelation temperature of agar of 40 °C) had a denser double network structure and higher mechanical strength than that formed at 0 °C due to inhibition of diffusion of Ca2+ as salt bridges for Fblg. The hydrophilic drugs were loaded in the meshes of the composite gels and their release was determined by the structure of the composite gel networks, whereas the hydrophobic drugs were loaded by attaching to the Fblgs in the composite gels and their release was determined by the loading ability and strength of the gels. The study not only provided a new idea for the preparation and application of polysaccharide-protein fiber composite hydrogels, but also provided insights for improving the efficiency of drug carriers.

Robustly and Intrinsically Stretchable Ionic Gel-Based Moisture-Enabled Power Generator with High Human Body Conformality.

Direct harvesting of energy from moist air will be a promising route to supply electricity for booming wearable and distributed electronics, with the recent rapid development of the moisture-enabled electricity generator (MEG). However, the easy spatial distortion of rigid MEG materials under severe deformation extremely inconveniences the human body with intense physical activity, seriously hindering the desirable applications. Here, an intrinsically stretchable moisture-enabled electricity generator (s-MEG) is developed based on a well-fabricated stretchable functional ionic gel (SIG) with a flexible double-network structure and reversible cross-linking interactions, demonstrating stable electricity output performance even when stretched up to 150% strain and high human body conformality. This SIG exhibits ultrahigh tensile strain (∼600%), and a 1 cm × 1 cm SIG film-based s-MEG can generate a voltage of ∼0.4 V and a current of ∼5.7 μA when absorbing water from humidity air. Based on the strong adhesion and the excellent interface combination of SIG and rough fabric electrodes induced by the fabrication process, s-MEG is able to realize bending or twisting deformation and shows outstanding electricity output stability with ∼90% performance retention after 5000 cycles of bending tests. By connecting s-MEG units in series or parallel, an integrated device of "moisture-powered wristband" is developed to wear on the wrist of humans and drive a flexible sensor for tracking finger motions. Additionally, a comfortable "moisture-powered sheath" based on s-MEGs is created, which can be worn like clothing on human arms to generate energy while walking and flexing the elbow, which is promising in the field of wearable electronics.

Self‐powered sensor based on compressible ionic gel electrolyte for simultaneous determination of temperature and pressure

AbstractThe simultaneous detection of multiple stimuli, such as pressure and temperature, has long been a persistent challenge for developing electronic skin (e‐skin) to emulate the functionality of human skin. Meanwhile, the demand for integrated power supply units is an additional pressing concern to achieve its lightweightness and flexibility. Herein, we propose a self‐powered dual temperature–pressure (SPDM) sensor, which utilizes a compressible ionic gel electrolyte driven by the potential difference between MXene and Al electrodes. The SPDM sensor exhibits a rapid and timely response to changes in pressure‐induced deformation, while exhibiting a slow and hysteretic response to temperature variations. These distinct response characteristics enable the differentiation of current signals generated by different stimuli through machine learning, resulting in an impressive accuracy rate of 99.1%. Furthermore, the developed SPDM sensor exhibits a wide pressure detection range of 0–800 kPa and a broad temperature detection range of 5–75°C, encompassing the environmental conditions encountered in daily human life. The dual‐mode coupled strategy by machine learning provides an effective approach for temperature and pressure detection and discrimination, showcasing its potential applications in wearable electronics, intelligent robots, human–machine interactions, and so on.

Ti3C2Tx Filled in EMIMBF4 Semi-Solid Polymer Electrolytes for the Zinc-Metal Battery.

Zinc-ion batteries (ZIBs) are promising candidates for safe energy storage applications. However, undesirable parasitic reactions such as dendrite growth, gas evaluation, anode corrosion, and structural damage to the cathode under an acidic microenvironment severely affected cell performance. To resolve these issues, an MXene entrapped in an ionic liquid semi-solid gel polymer electrolyte (GPE) composite was explored. The molecular-level mixing of poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF), zinc trifluoromethanesulfonate (Zn(OTF)2), 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIBF4) ionic liquid, and Ti3C2Tx MXene provided a controlled Zn2+ shuttle toward the anode/cathode. Ti3C2Tx/EMIBF4/Zn(OTF)2/PVHF exhibited a breaking strength of 0.36 MPa with an associated extension of 23%. The Zn//Ti3C2Tx/EMIBF4/Zn(OTF)2/PVHF//Zn symmetric cell with continuous zinc plating/stripping exhibited excellent Zn2+ ion mobility toward the anode and cathode without undesired reactions. This was confirmed by post-mortem analysis after a symmetric cell compatibility test. The as-prepared GPE with a Na3V2(PO4)3 (NVP) cathode exhibited a high chemical diffusion coefficient of 1.14 × 10-7. It also showed an outstanding reversible capacity of 89 mAh g-1 at C/10 with an average discharge plateau voltage of 1.45 V, cycle durability, and controlled self-discharge. These results suggested that the Zn2+ ions in the Ti3C2Tx/EMIBF4/Zn(OTF)2/PVHF composite are reversibly labile in the anode and cathode directions.

A Mini-Review: Fabrication of Polysaccharide Composite Materials Based on Self-Assembled Chitin Nanofibers.

This mini-review presents the fabrication methods for polysaccharide composite materials that employ self-assembled chitin nanofibers (ChNFs) as functional components. Chitin is one of the most abundant polysaccharides in nature. However, it is mostly not utilized because of its poor feasibility and processability. Self-assembled ChNFs are efficiently obtained by a regenerative bottom-up process from chitin ion gels using an ionic liquid, 1-allyl-3-methylimodazolium bromide. This is accomplished by immersing the gels in methanol. The resulting dispersion is subjected to filtration to isolate the regenerated materials, producing ChNF films with a morphology defined by highly entangled nanofibers. The bundles are disintegrated by electrostatic repulsion among the amino groups on the ChNFs in aqueous acetic acid to produce thinner fibers known as scaled-down ChNFs. The self-assembled and scaled-down ChNFs are combined with other chitin components to fabricate chitin-based composite materials. ChNF-based composite materials are fabricated through combination with other polysaccharides.

Regulatory and enhancement mechanism of a micro-nano material of sodium polystyrene sulfonate on the electro-responsive fatigue resistance of ion gel artificial muscles by cross-linking reaction

The Ion Gel Artificial Muscle (IGAM) is an emerging electro-responsive chemical actuator that holds significant potential for flexible actuation. This paper investigates the regulatory and enhancement mechanism of Sodium Polystyrene Sulfonate (PSS) on the electro-responsive fatigue resistance of IGAM by cross-linking with varying amounts of PSS, aiming to achieve high performance and durability. The study is conducted based on control variables and proposes four primary evaluation metrics. The results indicated that the optimal PSS amount of 0.75 mL yielded the highest values for peak difference (32.4 mN/g), response speed of output force density (0.07818 mN/g·s), and operating life of the IGAM (10,800 s). Additionally, under the excitation of short time reversible voltage, the quasi-impulse density of IGAM reached 10915 mN·s/g. Furthermore, the elastic modulus and internal resistance were found to be the lowest at 27.2 MPa and 1.55 Ω, respectively, while the area-specific capacitance increased to 400 nF/cm2. This phenomenon occurred due to the protonation of the sulfonyl groups, which were highly electronegative, on the PSS molecule. As a result, cross-linking hydrogen bonds were formed with the sodium alginate (SA) molecule, leading to the wrapping of its network and the formation of a regular three-dimensional ion gel network inside the IGAM. Both PSS and SA were polyanionic electrolytes, capable of increasing the number of anions present. This, in turn, facilitates the migration of hydrated cations within the IGAM, thereby enhancing its electro-responsive performance to suit various circumstances.

Low voltage driven microlens array based on ionic liquid doped polyvinyl chloride gels

Electrically responsive polyvinyl chloride (PVC) gels represent promising candidates for fabricating lenses with adjustable focal lengths. However, their practical use has been hampered by the elevated voltage requirements. In order to lower the driving voltage of PVC gels-based microlens array (MLA), trace ionic liquid (IL) −1-butyl-3-methylimidazole hexafluorophosphate ([BMIM]PF6) was doped. We employed a ring-array patterned electrode for the fabrication of PVC gels-based microlens arrays (MLAs). Our investigation revealed that the operating voltage for PVC gels-based MLAs doped with 0.01 wt% [BMIM]PF6 was nearly 1/22 of that required for MLAs created using undoped PVC gels. In the case of a microlens featuring a 250 μm aperture, the focal length varies from 4.2 mm to 2.5 mm as the voltage ranges from 5 V to 7 V. Importantly, this voltage range remains below the established safe limit for human exposure and obviates the need for intricate circuitry during manufacturing. Moreover, the extent of focal length variation can be expanded by augmenting the film thickness. Our approach offers valuable technical support for advancing the practical applications of PVC gel-based MLAs.

Fabrication and Therapeutic Process of a Green Silver-Nanoparticle-Embedded Mucilage Microsphere for Pathogenic-Bacteria-Infected Second-Degree Burn and Excision Wounds.

Multidrug-resistant bacteria are a serious problem in biomedical applications that decrease the wound healing process and increase the mortality rate. Therefore, in this study, we have prepared a green-synthesized silver-nanoparticle-encapsulated mucilage microsphere (HMMS@GSNP) from Hibiscus rosa sinensis leaves and applied it to pathogen-infected burn and excision wounds. Biophysical properties like size, polydispersity index, absorbance capacity, and drug release were measured by different techniques like field-emission scanning electron microscopy, dynamic light scattering, swelling ratio, etc. The strong antibacterial activity of a HMMS@GSNP microsphere was measured by minimum inhibitory concentration assay, minimum bactericidal concentration assay, and agar well diffusion methods. The HMMS@GSNP microsphere enhanced the cell viability, cell proliferation, migration, antioxidant, and antiinflammation activity compared to untreated GSNP and HMMS, as quantified by MTT assay, BrdU assay, scratch wound assay, reactive oxygen species scavenging assay, and Western blot analysis, respectively. In the in vivo experiment, we used a methicillin-resistant Staphylococcus aureus bacteria-infected, burn-and-excision-wound-created male BALB/c mice model. The HMMS@GSNP-treated burn-and-excision-wound-infected mice showed significant results compared to other groups (untreated, Silverex Ionic Gel, AgNO3, HMMS, and GSNP), and the mice tissues were utilized for bacteria count, immunoblot analysis, histological studies, and real-time polymerase chain reaction. Thus, the HMM@GSNP microsphere is an excellent therapeutic material that can be used as a topical agent for the management of chronic wound therapy.

Tunable H-bond effects enabled ionic conductive gels with high stretchability, transparency, self-adhesion and wide environmental tolerance for e-skin

It is a high demand but a great challenge to construct all-in-one ionic conductive hydrogels with excellent mechanical performances, transparency, self-adhesion, conductivity and environmental tolerance. Herein, a versatile gel platform was developed via a facile and rapid photopolymerization of acrylic acid (AA) in deep eutectic solvent (DES) with multiple roles simultaneously as water-free solvent, ionic conductor, regulator of hydrogen bond density. Benefiting from the formed crosslinking networks including covalently cross-linked polymer network and multiple dynamic interactions, the resultant PAA-DES gels exhibited high stretchability of 884.7 ± 4.9%, toughness of 31.2 ± 1.4 MJ/m3, fatigue resistance and recovery ability, transparency of 93%, self-adhesive strength of 472 kPa. Moreover, the inherent advantages of DES enabled the gels with good ionic conductivity (2.5 ± 0.2 mS/cm), wide working window and biocompatibility. The PAA-DES as self-adhesive ionic sensors not only possessed wide strain range (∼400%) and stability, but also displayed excellent humidity (30–80%), temperature (−40–60 °C), and sweat tolerance which could precisely and steadily discern and monitor human motions and weak physiological signals. Thus, this work not only provides a strategy to construct all-in-one ionic conductive gels with high elasticity, fatigue resilience, transparency, self-adhesion and wide environmental tolerance, but also exploits versatile platform for intelligent gel sensor and e-skin.