Tough Hydrogels Research Articles

Predicting Fatigue Damage in Hydrogels Through Force-Induced Luminescence Enhancement.

Fatigue damage of polymers occurs under long-term load cycling, resulting in irreversible fracture failure, which is difficult to predict. The real-time monitoring of material fatigue damage is of great significance. Here, tough hydrogels are prepared with force-induced confined luminescence enhancement of carbonated polymer quantum dot(CPD) clusters to realize the visualization of fracture process and the monitoring of fatigue damage. The enhanced interactions induced by force between the clusters and the polymer in the confined space inhibit the non-radiative leaps and promote the radiative leaps to quantify the fatigue damage into optical signals. Rigid CPDs with abundant active sites on the surface can form dynamic reversible bonds with polymer and dissipate stress concentration, which significantly enhances the crack propagation strain (8000%) and fracture energy (26.4kJ m-2) of hydrogels. CPDhydrogelshave a wide range of applications in novel information encryption and luminescent robotics.

A multifunctional and tough lotus root starch-based bio-photonic hydrogel for stretchable fabric pattern color change and water rewriting.

Photonic crystal hydrogels (PCHs) are innovative materials that translate imperceptible deformations and humidity changes into visible colors, broadening the applications of photonics in bioengineering and smart materials. To overcome poor mechanical properties of traditional PCHs limited by weak intermolecular forces, we designed a PCH with a dual-network framework comprising N-isopropylacrylamide-co-acrylamide (NIPAM-co-AM) and biomass lotus root starch (LR). Since LR is rich in hydroxyl groups, it can undergo molecular linkage entanglement with the NIPAM-co-AM hydrogel matrix, forming hydrogen bonds that significantly enhance the mechanical properties of the PCH. We have prepared PCH films capable of conveying multidimensional information about the extent and distribution of transient deformation by encapsulating magnetic photonic crystal microspheres (MPCMs) within a hydrogel matrix. The PCH films were found to have ultrafast response time (< 10 s), full-color tunable range, high spatial resolution, excellent mechanical toughness (tensile up to 0.17 MPa) and sensitivity (2.52 nm %-1), and were able to sense relative humidity (RH) from 11 % to 98 %. Equipped with a dynamically reconfigurable lattice, this dual-responsive (tensile/humidity) PCH not only facilitates the creation of water-rewritable photonic films but also holds promise for integration into structural color elastic fabrics, thereby presenting novel prospects for smart textile applications.

Multi-functional Gleditsia sinensis galactomannan-based hydrogel with highly stretchable, adhesive, and antibacterial properties as wound dressing for accelerating wound healing

Design and development of a multifunctional wound dressing with self-healing, adhesive, and antibacterial properties to attain optimal wound closure efficiency are highly desirable in clinical applications. Nevertheless, conventional hydrogels face significant barriers in their mechanical strength, adhesive performance, and antibacterial properties. Herein, a tough hydrogel based on aldehyde-grafted galactomannan was synthesized through radical copolymerization and Schiff base reaction, incorporating hyaluronic acid, acrylamide, and the zwitterionic monomer to create a multi-crosslinked structure. The multiple crosslink structure pattern consisting of multiple hydrogen bonding, ionic interactions, reversible Schiff bases bonds, and molecular chain entanglement endowed this hydrogel with multiple functionalities, including high tensile strength (25 kPa), tensile strain (2200 %), toughness (391.59 kJ/m3), and Young's modulus (9.77 kPa). The presence of catechol groups and zwitterionic groups endow hydrogels with outstanding adhesion strength (42.21 kPa), which satisfied the adhesive demand for the ample motion of specific areas. The zwitterionic monomer provided long-lasting antibacterial properties and promoted migration and growth of negatively charged cells, capable of establishing efficient antibacterial barriers and serving as wound dressing. The in vivo and vitro experiments manifested that the optimized hydrogel demonstrated an inconspicuous inflammatory response, facilitating rapid healing of full-thickness skin wound in rat models. Therefore, this work provides a promising strategy and an ideal candidate for wound healing dressings in treating infected skin wounds.

Potential Environmental Application of a Tough and Temperature-Responsive Nanocomposite Hydrogel Based on Poly(N-Isopropylacrylamide-co-Sodium Methacrylate) and Clay

Potential Environmental Application of a Tough and Temperature-Responsive Nanocomposite Hydrogel Based on Poly(N-Isopropylacrylamide-co-Sodium Methacrylate) and Clay

Continuous Phase Separation Induced Tough Hydrogel Fibers with Ultrahigh Conductivity for Multidimensional Soft Electronics

AbstractConductive hydrogel fibers exhibit great potential in soft robots, bioelectronics, and human–machine interfaces due to the unique combination of electrical conductivity, high water content, tissue‐like mechanical properties, and 1D structure. Despite significant advances in hydrogel technologies, the typical conductive hydrogel fibers show low conductivity (&lt;10 S cm−1), weak mechanical properties, and water stability, which makes it challenging to satisfy the requirements of practical applications. Here, a facile strategy is proposed to construct hydrogel fibers with ultrahigh conductivity and toughness by exploiting the synergistic effects of freezing‐thawing, salting‐out, and drying‐annealing. The continuous phase separation induced by the combined processes results in hierarchical structures, promoting the formation of interconnected conductive networks and increasing the fiber's crystallinity and crystal domain size. The prepared conductive hydrogel fibers exhibited ultrahigh conductivity (≈958 S cm−1), excellent mechanical properties (strength (≈6.2 MPa), stretchability (&gt;300%), and toughness (≈10 MJ m−2)), high water content (≈75%), outstanding water stability, and fatigue resistance properties. In addition, the processibility of conductive hydrogel yarns and fabrics are demonstrated and their potential application in bioelectronics. Overall, this work presents a preparation strategy for conductive hydrogel fibers, which will facilitate the advancement of soft electronics and may inspire structural construction in other polymers.

A Review of Advanced Hydrogel Applications for Tissue Engineering and Drug Delivery Systems as Biomaterials

Hydrogels are known for their high water retention capacity and biocompatibility and have become essential materials in tissue engineering and drug delivery systems. This review explores recent advancements in hydrogel technology, focusing on innovative types such as self-healing, tough, smart, and hybrid hydrogels, each engineered to overcome the limitations of conventional hydrogels. Self-healing hydrogels can autonomously repair structural damage, making them well-suited for applications in dynamic biomedical environments. Tough hydrogels are designed with enhanced mechanical properties, enabling their use in load-bearing applications such as cartilage regeneration. Smart hydrogels respond to external stimuli, including changes in pH, temperature, and electromagnetic fields, making them ideal for controlled drug release tailored to specific medical needs. Hybrid hydrogels, made from both natural and synthetic polymers, combine bioactivity and mechanical resilience, which is particularly valuable in engineering complex tissues. Despite these innovations, challenges such as optimizing biocompatibility, adjusting degradation rates, and scaling up production remain. This review provides an in-depth analysis of these emerging hydrogel technologies, highlighting their transformative potential in both tissue engineering and drug delivery while outlining future directions for their development in biomedical applications.

Poly(ionic liquid) functionalization: A general strategy for strong, tough, ionic conductive, and multifunctional polysaccharide hydrogels toward sensors

Poly(ionic liquid) functionalization: A general strategy for strong, tough, ionic conductive, and multifunctional polysaccharide hydrogels toward sensors

Laponite-Enabled Freeform Manufacturing of Tough Hydrogels with Colorimetric pH Sensitivity

Laponite-Enabled Freeform Manufacturing of Tough Hydrogels with Colorimetric pH Sensitivity

Super Strong and Tough PVA Hydrogel Fibers Based on an Ordered‐to‐Disordered Structural Construction Strategy Targeting Artificial Ligaments

AbstractHydrogels with high strength, high modulus, and high toughness have great application potential in the field of artificial human load‐bearing tissues, but the preparation of materials with the above high performance is still a huge challenge. In this paper, a structural construction strategy of ordered‐to‐disordered (OTD) transition is proposed to obtain hydrogel fibers with high strength, high modulus, and high toughness. The structural construction strategy of OTD refers to the ordered‐to‐disordered transition of molecular segments in PVA polymer fibers through swelling and subsequent salting‐out treatment, while still maintaining the general order of the entire polymer chain. PVA molecular chain crystallites provide physical crosslinking to stabilize the structure. The results show that the elongation at break of the hydrogel fiber can reach 257%). The strength reaches 190.04 MPa, which is more than 4 times higher than that of human ligaments. The modulus reaches 137.31 MPa, which perfectly matches the human ligaments, and the toughness can reach 100.61 MJ m−3. In addition, it has stable mechanical properties in liquid environment and excellent biocompatibility, which has great application potential in the field of artificial ligaments. This OTD structural construction strategy provides a facile approach to achieving hydrogel fibers with desired mechanical properties.

Multiresponsive Color-Changing and Tough Hydrogels Enabled by Self-Assembled Epoxy Oligomer Microspheres.

The fabrication process of hydrogels often incorporates various strategies to achieve multiple responses and enhance strength, which always make the procedure complex and even hinder the incorporation. Here, we develop a facile and flexible method to simultaneously achieve multiresponsive color-changing and tough properties in hydrogels by introducing epoxy oligomer microspheres (DEPMS) to hydrophobic association (HA) hydrogels. DEPMS is responsive to both pH and solvents, showing color changes due to conversion to a conjugated structure. The obtained DEPMS composite hydrogels could demonstrate diverse color-changing patterns by simply adjusting the components and pH of the solvents. Meanwhile, amphiphilic DEPMS helps to disperse hydrophobic regions of the HA hydrogel, resulting in more uniform cross-linking and thereby contributing to the enhanced mechanical properties. The tensile strength and toughness of the composite hydrogels could be easily adjusted and reach 1.00 MPa and 11.18 MJ m-3, respectively. This work provides an approach to the design of multiple responsive and tough hydrogels while offering insights into the recycling of waste epoxy resins.

Hydrogel Films with Impact Resistance by Sacrificial Micelle-Assisted-Alignment.

Various strategies are developed to engineer aligned hierarchical architectures in polymer hydrogels for enhanced mechanical performance. However, chain alignment remains impeded by the presence of hydrogen bonds between adjacent chains. Herein, a facile sacrificial micelle-assisted-alignment strategy is proposed, leading to well-aligned, strong and tough pure chitosan hydrogels. The sacrificial sodium dodecyl sulfate micelles electrostatically interact with the protonated chitosan chains, enabling chain sliding and alignment under uniaxial forces. Subsequently, sacrificial micelles can be easily removed via NaOH treatment, causing the reforming of H-bond in the chain networks. The strength of the pure chitosan hydrogels increases 140-fold, reaching 58.9±3.4MPa; the modulus increases 595-fold, reaching 226.4±42.8MPa. After drying-rehydration, the strength and modulus further rise to 70.3±2.4 and 403.5±76.3MPa, marking a significant advancement in high-strength pure chitosan hydrogel films. Furthermore, the designed multiscale architectures involving enhanced crystallinity, well-aligned fibers, strong interfaces, robust multilayer Bouligand assembly contribute to the exact replica of lobster underbelly with impact resistance up to 6.8±1.0kJ m-1. This work presents a promising strategy for strong, tough, stiff and impact-resistant polymer hydrogels via well-aligned hierarchical design.

Tough gelatine hydrogels reinforced with silk fibroin nanofiber

Gelatine hydrogels exhibit potential as biomaterials such as wound-healing materials, artificial organs, scaffolds for cell culture and drug delivery systems because of their good biocompatibility. However, their practical applications are limited by their poor mechanical properties and high degradability. In this study, mechanically fibrillated silk fibroin (fibroin nanofibers; FNF) was used to reinforce gelatine hydrogels. The resulting gelatine hydrogels with FNF exhibited enhanced toughness compared to those reinforced with conventional aqueous regenerated fibroin (RF), which were prepared by treatment with a highly concentrated LiBr solvent or a neat gelatine hydrogel while retaining their softness. The average pore size of the gelatine hydrogel was 2.2 μm, while the gelatine hydrogel containing 25 % FNF expanded to 6.7 μm. A web-like network was formed between the pores. The addition of FNF increased the relative β-sheet contents in the hydrogels to 60.3 %, suggesting that this may have caused structural changes such as increased crystallinity for gelatine-derived proteins. Furthermore, the addition of FNF inhibited the rapid enzymatic degradation of gelatine hydrogels. FNF, which can be easily prepared in water, is a safe material for both the environment and living organisms and holds promise as a biomaterial in the future.

Tough and anisotropic Janus hydrogel for tendon injury repair with controlled release of bFGF in tendon microenvironment

To address the high complexity and challenging nature of large-scale tendon injury repair, an innovative Janus structured hydrogel patch (JAHP@bFGF) was designed in this study. The patch combines microenvironmental responsiveness with efficient repair function, aiming to optimise and accelerate the tendon healing process. The outer layer is a PVA/SA/Na3Cit hydrogel with excellent mechanical properties, protein resistance, and low friction, which provides firm support to the tendon and reduces adhesions to ensure the recovery of gliding function. The inner layer of TCSB@bFGF microgel responds intelligently to changes in the microenvironment, precisely regulates the release of bFGF, promotes cell proliferation and migration, accelerates tissue regeneration, and has high adhesion strength and antimicrobial properties, which significantly reduces the risk of postoperative infection. Experimental results show that JAHP@bFGF significantly optimises the healing process, accelerates the repair speed and improves the repair quality under simulated large-scale tendon injury conditions. The unique Janus surface design and the intelligent drug release function, in synergy, not only bring new hope to patients with large-scale tendon injuries, but also provide an important reference for the application of biomedical materials in the repair of complex tissues, which heralds the arrival of the era of more efficient and personalised tendon repair.

3D Printing of Tough Hydrogel Scaffolds with Functional Surface Structures for Tissue Regeneration.

Hydrogel scaffolds have numerous potential applications in the tissue engineering field. However, tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties. Inspired by Chinese ramen, we propose a universal fabricating method (printing-P, training-T, cross-linking-C, PTC & PCT) for tough hydrogel scaffolds to fill this gap. First, 3D printing fabricates a hydrogel scaffold with desired structures (P). Then, the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance (T). Finally, the training results are fixed by photo-cross-linking processing (C). The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66MPa (622-fold untreated) and have excellent biocompatibility. Furthermore, this scaffold possesses functional surface structures from nanometer to micron to millimeter, which can efficiently induce directional cell growth. Interestingly, this strategy can produce bionic human tissue with mechanical properties of 10kPa-10MPa by changing the type of salt, and many hydrogels, such as gelatin and silk, could be improved with PTC or PCT strategies. Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers, blood vessels, and nerves within 4weeks, prompting the rapid regeneration of large-volume muscle loss injuries.

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.

MXene-based self-adhesive, ultrasensitive, highly tough flexible hydrogel pressure sensors for motion monitoring and robotic tactile sensing

With the rapid development of artificial intelligence and human–computer interaction fields, wearable electronic devices represented by flexible pressure sensors have a wider range of application scenarios. In this paper, we used a composite hydrogel made by one-pot polymerization using a combination of acrylamide (AM), sodium carboxymethyl cellulose (CMC), dopamine (DA), and MXene (Ti3C2Tx). The composite hydrogel has the advantages of self-adhesion, high sensitivity, large detection range (0–500 kPa), low detection limit, high toughness (compression > 90 %), stability (more than 6700 s) and other advantages of hydrogel flexible pressure strain sensor. Sodium carboxymethyl cellulose (CMC), as a multifunctional thickener and gelling agent, significantly improves rheological properties and viscosity in hydrogels, forms crosslinked structures to enhance mechanical properties and provides reliable toughness for pressure sensors. Dopamine (DA), which is rich in catechol groups, can adhere to the material surface through oxidative polymerization to enhance bond strength. Hydrogel pressure sensors for human motion detection can accurately track joint movement, respond sensitively to changes in knocks and touches, and display specific characters such as Morse code. The technology extends to robotic systems, where pressure-activated electrical signals are used to control robot movements. Therefore, it has a very promising application in the field of human–computer interaction, human-body movement signal detection, etc. PAM/CMC/DA/MXene hydrogel pressure sensors have excellent mechanical, electrical, and adhesion properties, which provide a more reliable solution for the fields of flexible wearable e-skin, human–computer interaction, and tactile sensing.

Self-Polymerized Tough and High-Entanglement Zwitterionic Functional Hydrogels.

Zwitterionic hydrogels exhibit great potential in biomedical applications due to their antifouling properties and biocompatibility. However, the single-network structure of pure zwitterionic hydrogels leads to a low toughness and strength, limiting their application in biomedical fields. In this work, a high entanglement sulfobetaine methacrylate-dopamine hydrogel (SBMA-DA-PE) with low cross-linker content and high monomer concentration is prepared by using a dopamine oxidative radical polymerization method. Compared to a regular zwitterionic hydrogel, the SBMA-DA-PE hydrogel exhibits a 5-fold increase in tensile fracture stress and a 10-fold increase in compressive fracture stress. The SBMA-DA-PE hydrogel possesses excellent mechanical properties (the maximum compressive stress ≥4.85MPa, the maximum compressive strain ≥90%). Besides, the non-covalent interactions between catechol or ortho-quinones within the SBMA-DA-PE hydrogel, combined with strong intermolecular electrostatic interactions, endow the SBMA-DA-PE hydrogel with great self-healing capabilities and fatigue resistance. The SBMA-DA-PE hydrogel demonstrates low swellability and possesses good antifouling properties. Furthermore, the good printability and conductivity of the tough SBMA-DA-PE hydrogel endows it with new possibilities for developing biological 3D scaffolds and electronic devices. Overall, this work provides new insights into the preparation of zwitterionic hydrogels with high mechanical strength and multi-functionality for biomedical applications.

Room temperature shape self-adjustable tough hydrogel based on multi-physical crosslinking

Room temperature shape adjustable hydrogels (rtSAH) can be (re)processed into different stable shapes at ambient conditions, making them appealing for various applications. However, elastomer-like and mechanically tough rtSAH is hard to obtain because of the elastic recovery force that prevents a deformed new shape from being fixed. Herein, we demonstrate a supramolecular elastic rtSAH having high tensile strength (2.6 MPa) and large strain at break (1770 %), whose network structure is designed to rely on a combination of strong and weak non-covalent interactions through three types of physical crosslinking: host–guest interaction, hydrogen bonding and coordination interaction. When deformed at room temperature and held in that state for sufficient time, the hydrogel adapts to a stable new shape while remaining elastic. The reconstruction of the dynamic Fe3+-carboxylate coordination interaction in the deformed hydrogel is the key to self-locking the new shape with stored elastic energy and enabling the shape memory function. Exposure the rtSAH to UV light or an acid solution disrupts the coordination crosslinking and allows the hydrogel to recover its initial shape. The demonstrated structural design represents an effective strategy to develop all-physically crosslinked shape memory hydrogels whose shapes can be reprocessed and self-locked at room-temperature.

Fabrication of Strong Tough Hydrogels Inspired by the Hydration-Flexibilization Process of Discinisca tenuis Shells

Fabrication of Strong Tough Hydrogels Inspired by the Hydration-Flexibilization Process of Discinisca tenuis Shells

Bioinspired Bouligand-Structured Cellulose Nanocrystals/Poly(vinyl alcohol) Composite Hydrogel for Enhanced Impact Resistance.

Impact-protective materials are gaining importance because of the widespread occurrence of impact damage. Hydrogels have emerged as promising candidates owing to their lightweight and flexible nature. However, achieving soft impact-resistant hydrogels with exceptional stiffness, strength, and toughness remains a challenge. Inspired by the Bouligand structure found in the smasher dactyl club of stomatopods, we propose a straightforward multiscale hierarchical structural design strategy. This strategy integrates self-assembly and salting-out techniques to enhance the impact resistance of soft hydrogels. Rigid cellulose nanocrystals (CNCs) self-assemble into Bouligand-like structures within soft poly(vinyl alcohol) (PVA) matrix via supramolecular interactions. This rational structural design combines the CNC Bouligand structure with a cross-linked network of soft PVA crystalline domains, resulting in a composite hydrogel with impressive mechanical properties: high tensile fracture strength (30.2 MPa), elastic modulus (62.7 MPa), and fracture energy (75.6 kJ m-2), surpassing those of other tough hydrogels. Moreover, the multiscale hierarchical structure facilitates various energy dissipation mechanisms, including crack twisting, tortuous crack paths, and PVA chain orientation, resulting in notable force attenuation (80.4%) in the composite hydrogel. This biomimetic design strategy opens new avenues for developing soft and lightweight impact-resistant materials.