Tunable Mechanical Properties Research Articles

Cytocompatible Hydrogels with Tunable Mechanical Strength and Adjustable Swelling Properties through Photo-Cross-Linking of Poly(vinylphosphonates).

Herein, the synthesis, characterization, and application of a novel synthetic hydrogel based on the photoinitiated cross-linking of poly(vinylphosphonates) is presented. First, statistical copolymers with adjustable ratios of the monomers diallyl vinylphosphonate (DAlVP) and diethyl vinylphosphonate (DEVP), as well as different molecular weights, were obtained via rare earth metal-mediated group-transfer polymerization (REM-GTP) while maintaining narrow polydispersities. The copolymers were cross-linked by applying photoinitiated thiol-ene click chemistry (λ = 365 nm). The network formation was monitored via oscillatory rheology coupled with UV-irradiation, revealing the high spatiotemporal control of the reaction. Moreover, the equilibrium storage moduli of poly(vinylphosphonate)-based hydrogels increased with a growing number of DAlVP units and upon application of a different cross-linker, which was additionally confirmed by nanoindentation experiments. In contrast, the water uptake of hydrogels decreased with higher DAlVP amounts in the corresponding hydrogels due to lower chain mobility and an overall increase in the hydrophobicity of the samples. Upon successful functionalization of P(DEVP-stat-DAlVP) copolymers with sodium 3-mercaptopropane-1-sulfonate, as indicated via 1H DOSY NMR, the respective cross-linked materials displayed a remarkable increase in the water uptake; thus, presenting highly hydrophilic gels with an apparent interplay between water uptake, cross-linking density, and functionalization degree. Finally, the purified hydrogels showed cytocompatibility and enabled cell adhesion of human umbilical artery smooth muscle cells (HUASMCs) after direct seeding. The materials further allowed the adhesion and growth of an endothelial layer, triggered no pro-inflammatory response as evidenced by cytokine release of M0 macrophages, and exhibited antibacterial properties toward S. aureus and E. coli.

Temporal evolution of mechanical properties in PDMS: A comparative study of elastic modulus and relaxation time for storage in air and aqueous environment

Polydimethylsiloxane (PDMS) is a soft, biocompatible polymer extensively employed in biomedical research, notable for its tunable mechanical properties achieved through cross-linking. While many studies have assessed the mechanical properties of PDMS utilizing macroscopic and microscopic methods, these analyses are often limited to freshly prepared samples. However, the mechanical properties of PDMS can be expected to change during prolonged exposure to water or air, such as interface polymer chain loosening or surface hardening, which are critical considerations in applications like cell culture platforms or microfluidic devices. This paper presents a comprehensive 10-day investigation of the evolution of PDMS surface mechanical properties through AFM-based nano-indentation. We focused on the most commonly utilized crosslinker-to-base ratios of PDMS, 1:10 (r10) and 1:20 (r20), under conditions of air and deionized water storage. For r10 samples, a hardening process was detected, peaking at 2.12 ± 0.35 MPa within five days for those stored in air and 1.71 ± 0.16 MPa by the third day for those immersed in water. During indentation, the samples displayed multiple contact points, suggesting the formation of distinct regions with varying mechanical properties. In contrast, r20 samples exhibited better stability, with an observed elastic modulus averaging 0.62 ± 0.06 MPa for air-stored and 0.74 ± 0.06 MPa for water-stored samples. Relaxation experiments, interpreted via the General Maxwell Model featuring two distinct component responses, a relatively consistent fast response τ1 (on the order of 10−1 s), and a more variable, slower response τ2 (on the order of 10 s), throughout the study period. The identification of two distinct relaxation times suggests the involvement of two disparate material property regimes in the relaxation process, implying changes in the surface material composition at the interface with air/water. These variations in mechanical properties could significantly influence the long-term functionality of PDMS in various biomedical applications.

Development of low-molecular-weight polysaccharide-based wound dressings for full-thickness cutaneous wound healing via coacervate formation

The development of polysaccharide-based wound dressings that are easy to prepare, adhere to tissue, adapt to diverse shapes and exhibit tunable mechanical properties holds significant clinical interest. This study introduced a simple spontaneous liquid-liquid phase separation technique employing low-molecular-weight and high polyion concentration of chitosan (CS) and hyaluronic acid (HA) to fabricate CS/HA coacervates. Upon increasing the molecular weight of chitosan from 7 kDa to 250 kDa, a transition in the CS/HA coacervates from liquid-like state to an elastic liquid and eventually to a solid-like state was observed. The resulting CS/HA coacervates demonstrated robust water resistance and adhesion to skin tissue. Notably, the molecular weight of chitosan significantly influenced the mechanical properties and hydration levels of the CS/HA coacervates. Moreover, in vivo studies using a full-thickness cutaneous defect model revealed that the CS/HA coacervates, prepared using 100 kDa chitosan, markedly accelerate wound healing. The coacervates' ease of preparation, wet adhesion, heterogeneous structure, suitability for irregularly shaped wounds, and exceptional wound healing promotion of the coacervates qualify them as an optimal wound dressing.

Toward mechanical proprioception in autonomously reconfigurable kirigami-inspired mechanical systems.

Mechanical metamaterials have recently been exploited as an interesting platform for information storing, retrieval and processing, analogous to electronic devices. In this work, we describe the design and fabrication a two-dimensional (2D) multistable metamaterial consisting of building blocks that can be switched between two distinct stable phases, and which are capable of storing binary information analogous to digital bits. By changing the spatial distribution of the phases, we can achieve a variety of different configurations and tunable mechanical properties (both static and dynamic). Moreover, we demonstrate the ability to determine the phase distribution via simple probing of the dynamic properties, to which we refer as mechanical proprioception. Finally, as a simple demonstration of feasibility, we illustrate a strategy for building autonomous kirigami systems that can receive inputs from their environment. This work could bring new insights for the design of mechanical metamaterials with information processing and computing functionalities. This article is part of the theme issue 'Origami/Kirigami-inspired structures: from fundamentals to applications'.

Nonlinear viscoelasticity of filamentous fungal biofilms of Neurospora discreta

The picture of bacterial biofilms as a colloidal gel composed of rigid bacterial cells protected by extracellular crosslinked polymer matrix has been pivotal in understanding their ability to adapt their microstructure and viscoelasticity to environmental assaults. This work explores if an analogous perspective exists in fungal biofilms with long filamentous cells. To this end, we consider biofilms of the fungus Neurospora discreta formed on the air-liquid interface, which has shown an ability to remove excess nitrogen and phosphorous from wastewater effectively. We investigated the changes to the viscoelasticity and the microstructure of these biofilms when the biofilms uptake varying concentrations of nitrogen and phosphorous, using large amplitude oscillatory shear flow rheology (LAOS) and field-emission scanning electron microscopy (FESEM), respectively. A distinctive peak in the loss modulus (G″) at 30–50 % shear strain is observed, indicating the transition from an elastic to plastic deformation state. Though a peak in G″ has been observed in several soft materials, including bacterial biofilms, it has eluded interpretation in terms of quantifiable microstructural features. The central finding of this work is that the intensity of the G″ peak, signifying resistance to large deformations, correlates directly with the protein and polysaccharide concentrations per unit biomass in the extracellular matrix and inversely with the shear-induced changes in filament orientation in the hyphal network. These correlations have implications for the rational design of fungal biofilms with tuneable mechanical properties.

Gelatin-based hydrogels with tunable network structure and mechanical property for promoting osteogenic differentiation

Osteoarthritis (OA) is a joint disease involving all joint components, including cartilage, calcified cartilage, and subchondral bone. The repair of osteochondral defects remains a significant challenge in orthopedics. Development of new strategies is essential for effective osteochondral injury repair. In this study, gelatin (Gel), polyethylene glycol diglycidyl ether (PEGDGE), hydroxyethyl cellulose (HEC) and chitosan (CS) were used to prepare semi-IPNs and IPNs hydrogels. Mechanical properties of Gel based hydrogels significantly improved with the semi-IPN and IPN structures. Tensile strength ranges from 238.7 KPa to 479.5 KPa, and its compressive strength ranges from 35.6 KPa to 112.7 KPa. Additionally, the stress relaxation rate increased with higher CS concentrations, ranging from 25 % to 35 %. The network structure of Gel-based hydrogels was a key factor in regulating stress relaxation. Viscoelasticity was adjusted by its network structures. Swelling and degradation behaviors of Gel based hydrogels were systematically investigated. Gel based hydrogels had good cytocompatibility. Both semi-IPN and IPN structures Gel based hydrogels could promote cell spreading and osteogenic differentiation. G10HEC1 and G10CS1 hydrogels show promise as candidates for osteochondral tissue regeneration, offering a new strategy for osteochondral tissue engineering.

A semi-conductive rigid polyurethane foam derived from kraft lignin polyol and a PEDOT: PSS coating

Rigid polyurethane foams (RPUF) are mainly used as thermal insulators materials. These materials are drawing the attention of the emerging sector of the Internet of Things (IoT) due to their features such as good chemical resistance, lightweight, and tunable mechanical properties. Yet, for IoT applications, the electrical conductivity of this type of materials should be increased substantially. To address this challenge, as well as the urgency to use renewable and sustainable resources, semi-conductive RPUF were synthesized using crude lignin-based polyol (LBP) doped with multi-walled carbon nanotubes (MWCNT) and coated with PEDOT: PSS, using the dip coating technique. The ensuing semi-conductive RPUF has low density (33–34 kg/m3), high electrical conductivity (in the order of magnitude of 10−5 S/m), and a stretchability enhancement of almost 50 % upon coating with PEDOT: PSS. Furthermore, the mechanical performance of RPUFs can be adjusted using MWCNT and fine tuning of the formulation. Lignin being an abundant natural aromatic polyol allows the partial replacement of fossil derived polyols in the production of RPUFs and its aromatic structure contributes to the thermal and mechanical stability of the ensuing foams.

Microstructure and properties controlling of Al-xGd alloys for thermal neutron absorbing

A novel lightweight thermal neutron absorbing Al-xGd alloy (x = 2.5, 5, and 10 wt.%) with tunable mechanical properties was fabricated by induction melting followed by a rolling process and an annealing treatment. During solidification, the Al3Gd phase predominantly formed and was distributed along grain boundaries. Cold rolling crushed and redistributed the Al3Gd phase throughout the matrix. Furthermore, the large deformation imposed on the material during cold rolling enhanced the work hardening effect and promoted dynamic recrystallization. The load transfer strengthening effect was influenced by the size, volume fraction, and distribution of the second phase. The spheroidization of the second phase increased rapidly and then remained stable during 5000 h long-term aging at 400°C. The thermal neutron absorbing performance of the Al-5Gd alloy is comparable to the 30%B4C/Al composite evaluated by Monte Carlo simulations. Furthermore, Al-5Gd alloy exhibited higher plasticity (> 20%). This novel Al-xGd alloy is a promising candidate for future lightweight thermal-neutron-absorbing materials.

Dynamic imine crosslinking for waterproof starch plastic with tunable mechanical properties

Starch-based plastics offer a potential solution to environmental pollution and can reduce the dependence on petroleum-based plastics. However, effectively preparing starch-based plastics with moisture resistance and high strength remains challenging. Herein, dialdehyde starch (DAS) with different degrees of oxidation was first synthesised. The molecular weight and crystallinity of DAS decreased depending on the aldehyde content, as determined through scanning electron microscopy, X-ray diffraction and molecular weight analyses. Subsequently, a sustainable starch plastic (DAS-DA) was prepared via the dynamic imine crosslinking of DAS with diamines. The influence of the degree of oxidation of DAS on the structure and properties of DAS-DA was systematically investigated. No linear relationship was observed between the tensile strength of DAS-DA and the aldehyde content of DAS. When the aldehyde content was 41.1 %, the resulting DAS41-DA exhibited optimal mechanical strength (27.8 MPa), exceeding that of most reported starch-based plastics. In addition, owing to the presence of imine crosslinking networks, DAS41-DA exhibited excellent water and solvent resistance (>60 days), good thermal stability (456 °C–462 °C) and excellent reprocessability and biodegradability. These findings provide a theoretical basis for the preparation of high-performance bioplastics from aldehyde-containing polysaccharides.

In-situ preparation of lanthanide luminescent MOF hydrogel for aldehyde detection☆

Metal-organic frameworks (MOFs) usually exist in the state of powder or crystal. When they are exposed to hydrophilic solvents, their structure will change and become unstable. Therefore, it is a challenge to construct MOF materials with tunable mechanical properties. Herein, we report in-situ growth lanthanide metal-organic framework (LnMOF) in sodium alginate (SA) and polyvinyl alcohol (PVA) hydrogel matrix. The prepared composite hydrogel not only displays characteristic lanthanide narrow-band emission under ultraviolet light, but also demonstrates excellent mechanical properties. The addition of LnMOF significantly enhances the compressive strength of the hydrogel (from 0.75 to 7.32 MPa). Furthermore, the composite hydrogel shows highly selective recognition of glutaraldehyde and gaseous formaldehyde at room temperature. The detection limits (LOD) of SP-EuMOF for glutaraldehyde and formaldehyde are 0.27 and 0.22 ppm, respectively. Based on these results, the LnMOF composite hydrogel is deemed to have significant potential as a fluorescent sensor for both glutaraldehyde and formaldehyde detection.

In-situ polymerized boehmite/ cashew gum/ polyvinyl alcohol/ polypyrrole blend nanocomposites with tunable structural, electrical, and mechanical properties for enhanced energy storage applications

This study describes the successful synthesis of boehmite (BHM) nanofiller-reinforced ternary blend nanocomposite films composed of polyvinyl alcohol (PVA), cashew gum (CG), and polypyrrole (PPy) using in-situ polymerization with water as the environmentally friendly solvent. The blend nanocomposites were characterized using Fourier-transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FE-SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). FTIR analysis revealed chemical bonding between BHM and the biopolymer matrix at1071 cm-1. FE-SEM images exhibited a uniform distribution of BHM nanofillers within the CG/PVA/PPy matrix, particularly at a 10 wt% concentration. The addition of BHM significantly enhanced the thermal stability and the glass transition temperature of the nanocomposites. The temperature-sensitive AC conductivity, activation energy, and dielectric properties were examined using an impedance analyzer. AC conductivity analysis revealed reduced activation energy (1.277 × 10⁻5 eV at 7 wt% BHM) and increased dielectric constant (from 565.28 to 4411.22). The ternary blend nanocomposite demonstrated a significant 60.2 % increase in tensile strength, reflecting enhanced force resistance, while hardness values ranged from 26 to 30, classifying the films as soft and flexible. Overall, the study highlights significant enhancements in the morphological, electrical, thermal, dielectric, and mechanical properties of the nanocomposite films, emphasizing their promising potential for energy storage applications.

Highly Stretchable, Transparent, Solvent-Resistant Multifunctional Ionogel with Underwater Self-Healing and Adhesion for Wearable Strain Sensors and Barrier-Free Information Transfer.

Ionogels with excellent deformability, high ionic conductivity, and a sensitive stimulus response have been widely used and rapidly developed in flexible wearable systems. However, previously reported ionogels are mainly limited to atmospheric environments applications and have difficulty meeting the requirements of solvent-resistant, self-healing, and adhesion properties in underwater environments. Herein, a multifunctional ionogel capable of underwater applications is prepared by one-step photoinitiated polymerization of a fluorine-containing monomer (2,2,3,4,4,4-hexafluorobutyl acrylate, HFBA) and acrylic acid (AA) in a hydrophobic ionic liquid ([EMIM][TFSI]). The dynamic physical interactions of hydrogen bonds and ionic dipoles endow the ionogel with remarkable transparency, tunable mechanical properties, and underwater self-healing properties. Moreover, the fluoropolymer matrix offers high resistance to water and various solvents and exhibits strong underwater adhesion on different substrates. Thus, the sensor based on the ionogel exhibits excellent sensing properties, including high sensitivity, fast response, and superior durability. In particular, the ionogel can be used as a wearable underwater sensor to perform barrier-free information transfer. This study provides a design idea for the development of underwater flexible strain sensors.

Accurate Crystal Structure Prediction of New 2D Hybrid Organic-Inorganic Perovskites.

Low-dimensional hybrid organic-inorganic perovskites (HOIPs) are promising electronically active materials for light absorption and emission. The design space of HOIPs is extremely large, as a variety of organic cations can be combined with different inorganic frameworks. This not only allows for tunable electronic and mechanical properties but also necessitates the development of new tools for in silico high throughput analysis of candidate materials. In this work, we present an accurate, efficient, and widely applicable machine learning interatomic potential (MLIP) trained on 86 diverse experimentally reported HOIP materials. This MLIP was tested on 73 experimentally reported perovskite compositions and achieves a high accuracy, relative to density functional theory (DFT). We also introduce a novel random structure search algorithm designed for the crystal structure prediction of 2D HOIPs. The combination of MLIP and the structure search algorithm reliably recovers the crystal structure of 14 known 2D perovskites by specifying only the organic molecule and inorganic cation/halide. Performing this crystal structure search with ab initio methods would be computationally prohibitive but is relatively inexpensive with the MLIP. Finally, the developed procedure is used to predict the structure of a totally new HOIP with cation (cis-1,3-cyclohexanediamine). Subsequently, the new compound was synthesized and characterized, which matches the predicted structure, confirming the accuracy of our method. This capability will enable the efficient and accurate screening of thousands of combinations of organic cations and inorganic layers for further investigation.

Polyvinyl Alcohol (PVA)-Based Hydrogels: Recent Progress in Fabrication, Properties, and Multifunctional Applications.

Polyvinyl alcohol (PVA)-based hydrogels have attracted significant attention due to their excellent biocompatibility, tunable mechanical properties, and ability to form stable three-dimensional networks. This comprehensive review explores the recent advancements in PVA-based hydrogels, focusing on their unique properties, fabrication strategies, and multifunctional applications. Firstly, it discusses various facile synthesis techniques, including freeze/thaw cycles, chemical cross-linking, and enhancement strategies, which have led to enhanced mechanical strength, elasticity, and responsiveness to external stimuli. These improvements have expanded the applicability of PVA-based hydrogels in critical areas such as biomedical, environmental treatment, flexible electronics, civil engineering, as well as other emerging applications. Additionally, the integration of smart functionalities, such as self-healing capabilities and multi-responsiveness, is also examined. Despite progress, challenges remain, including optimizing mechanical stability under varying conditions and addressing potential toxicity of chemical cross-linkers. The review concludes by outlining future perspectives, emphasizing the potential of PVA-based hydrogels in emerging fields like regenerative medicine, environmental sustainability, and advanced manufacturing. It underscores the importance of interdisciplinary collaboration in realizing the full potential of these versatile materials to address pressing societal challenges.

Mechanical and Biological Characterization of Ionic and Photo-Crosslinking Effects on Gelatin-Based Hydrogel for Cartilage Tissue Engineering Applications.

Articular cartilage degeneration poses a significant public health challenge; techniques such as 3D bioprinting are being explored for its regeneration in vitro. Gelatin-based hydrogels represent one of the most promising biopolymers used in cartilage tissue engineering, especially for its collagen composition and tunable mechanical properties. However, there are no standard protocols that define process parameters such as the crosslinking method to apply. To this aim, a reproducible study was conducted for exploring the influence of different crosslinking methods on 3D bioprinted gelatin structures. This study assessed mechanical properties and cell viability in relation to various crosslinking techniques, revealing promising results particularly for dual (photo + ionic) crosslinking methods, which achieved high cell viability and tunable stiffness. These findings offer new insights into the effects of crosslinking methods on 3D bioprinted gelatin for cartilage applications. For example, ionic and photo-crosslinking methods provide softer materials, with photo-crosslinking supporting cell stretching and diffusion, while ionic crosslinking preserves a spherical stem cell morphology. On the other hand, dual crosslinking provides a stiffer, optimized solution for creating stable cartilage-like constructs. The results of this study offer a new perspective on the standardization of gelatin for cartilage bioprinting, bridging the gap between research and clinical applications.

Dynamic mechanical and thermal analysis of 3D-printed ABS/POE blends for tunable mechanical properties

Dynamic mechanical and thermal analysis of 3D-printed ABS/POE blends for tunable mechanical properties

4D Printing Hybrid Soft Robots Enabled by Shape-Transformable Liquid Metal Nanoparticles.

In recent years, soft robotics has emerged as a rapidly expanding frontier research field that draws inspiration from the locomotion mechanisms of soft-bodied creatures in nature to achieve smooth and complex motion for diverse applications. However, the fabrication of soft robots with hybrid structures remains challenging due to limitations in material selection and the complex, multi-step processes involved in traditional manufacturing methods. Herein, a novel direct one-step additive manufacturing (3D printing) approach is introduced for the fabrication of hybrid robots composed of soft and rigid components for sophisticated tasks. Inspired by the shape-transformable liquid metal nanoparticles (LMNPs), a functional material toolkit with tuneable mechanical properties and deformability is developed by integrating differently shaped gallium-based nanoparticles (GNPs) into the 3D printing polymers. Then the direct printing of assembled or one-piece hybrid soft-rigid robots is presented through a single recipe of GNPs-integrated inks. This fabrication method enables precise control of the mechanical properties and shape memory properties within the hybrid structures of robot body with a customized structure design. Their capabilities are further demonstrated through the design and fabrication of hybrid robots as high-precision gripper, bioinspired motor, and hand rehabilitation device.

The effect of swelling/deswelling cycles on the mechanical behaviors of the polyacrylamide hydrogels

In practical applications, hydrogels experience swelling or deswelling in response to external stimuli, showcasing large deformation, tunable mechanical properties, and excellent biocompatibility. Previous studies focused on the effect of individual swelling or deswelling on the mechanical behaviors of hydrogels, neglecting the combined effects of both processes. The underlying mechanism of how the combined processes of swelling and deswelling affect the mechanical behaviors of hydrogels has not been systematically explored. To address this gap, polyacrylamide hydrogels with diverse initial compositions are prepared and subjected to controlled swelling-deswelling or deswelling-swelling cycles to achieve the same water content state. The mechanical properties of the hydrogel samples exposed to these cycles, including shear modulus, stretchability, Mullins effect, and fracture toughness, are experimentally evaluated and compared with those of as-prepared hydrogel samples without undergoing such cycles. Our findings reveal a significant reduction in stretchability, the Mullins effect, and fracture toughness of hydrogels exposed to either cycle. The extent of these reductions varies depending on the initial compositions of the hydrogels. This reduction in properties is primarily attributed to the rearrangement of hydrogel networks during these cycles, which becomes noticeable in hydrogels with network inhomogeneity. We also found that although the shear modulus of hydrogels varies after swelling-deswelling or deswelling-swelling cycles, it remains at relatively consistent levels compared to the as-prepared hydrogel. These findings suggest that the mechanical properties of hydrogels can be adjusted by optimizing the initial compositions and regulating the swelling-deswelling processing method. By studying the effects of swelling/deswelling cycles on the mechanical properties of hydrogels, we provide valuable insights for the application of hydrogels under dynamic environmental changes.

Multi-parametric Photoacoustic Imaging Combined with Acoustic Radiation Force Impulse Imaging for Applications in Tissue Engineering.

Tissue engineering is a dynamic field focusing on the creation of advanced scaffolds for tissue and organ regeneration. These scaffolds are customized to their specific applications and are often designed to be complex, large structures to mimic tissues and organs. This study addresses the critical challenge of effectively characterizing these thick, optically opaque scaffolds that traditional imaging methods fail to fully image due to their optical limitations. We introduce a novel multi-modal imaging approach combining ultrasound, photoacoustic, and acoustic radiation force impulse imaging. This combination leverages its acoustic-based detection to overcome the limitations posed by optical imaging techniques. Ultrasound imaging is employed to monitor the scaffold structure, photoacoustic imaging is employed to monitor cell proliferation, and acoustic radiation force impulse imaging is employed to evaluate the homogeneity of scaffold stiffness. We applied this integrated imaging system to analyze melanoma cell growth within silk fibroin protein scaffolds with varying pore sizes and therefore stiffness over different cell incubation periods. Among various materials, silk fibroin was chosen for its unique combination of features including biocompatibility, tunable mechanical properties, and structural porosity which supports extensive cell proliferation. The results provide a detailed mesoscale view of the scaffolds' internal structure, including cell penetration depth and biomechanical properties. Our findings demonstrate that the developed multimodal imaging technique offers comprehensive insights into the physical and biological dynamics of tissue-engineered scaffolds. As the field of tissue engineering continues to advance, the importance of non-ionizing and non-invasive imaging systems becomes increasingly evident, and by facilitating a deeper understanding and better characterization of scaffold architectures, such imaging systems are pivotal in driving the success of future tissue-engineering solutions.

Multi-Modal Sensing Ionogels with Tunable Mechanical Properties and Environmental Stability for Aquatic and Atmospheric Environments.

Ionogels have garnered significant interest due to their great potential in flexible iontronic devices. However, their limited mechanical tunability and environmental intolerance have posed significant challenges for their integration into next-generation flexible electronics in different scenarios. Herein, the synergistic effect of cation-oxygen coordination interaction and hydrogen bonding is leveraged to construct a 3D supramolecular network, resulting in ionogels with tunable modulus, stretchability, and strength, achieving an unprecedented elongation at break of 10800%. Moreover, the supramolecular network endows the ionogels with extremely high fracture energy, crack insensitivity, and high elasticity. Meanwhile, the high environmental stability and hydrophobic network of the ionogels further shield them from the unfavorable effects of temperature variations and water molecules, enabling them to operate within a broad temperature range and exhibit robust underwater adhesion. Then, the ionogel is assembled into a wearable sensor, demonstrating its great potential in flexible sensing (temperature, pressure, and strain) and underwater signal transmission. This work can inspire the applications of ionogels in multifunctional sensing and wearable fields.