Hydrogel Network Research Articles

Sliding-Induced Rehydration in Hydrogels for Restoring Lubrication and Anticreeping Capability.

Fluid exudation in cartilage under normal loading can be counteracted by a sliding-induced rehydration phenomenon, which has a hydrodynamic origin related to a wedge effect at the contact inlet. Similar to cartilage, hydrogels also exhibit tribological rehydration properties, and we mimic this phenomenon to restore hydration lubrication and overcome creeping. It occurs within a specific velocity range and is mainly dependent on the applied load and hydrogel network structures. Crucially, a certain velocity in the mixed lubrication regime can produce a hydrodynamic pressure peak at the wedge and drive the rehydration inflow to overcome the extrusion. At lower sliding velocities in the boundary lubrication regime, inflows are insufficient to counteract fluid exudation, whereas at higher velocities in the hydrodynamic lubrication regime, the inlet wedge effect would diminish. These results suggest that tribological rehydration offers a novel approach to enhancing load-bearing capacity and maintaining lubrication in the hydrogels.

Enhanced Biodegradation of Silk Fibroin Hydrogel for Preventing Postoperative Adhesion.

An absorbable adhesion barrier is a medical device that prevents postoperative adhesion and matches its biodegradation time with the regeneration period of its target tissues, which is important for antiadhesion effects. Physical hydrogels of Bombyx mori silk fibroin (SF) proteins are degradable in vivo. However, their biodegradation time is too long to exert antiadhesion effects. To shorten the biodegradation time of the SF hydrogels, we decreased the molecular weight (MW) of the SF proteins by alkaline treatment and prepared low-MW (LMW) SF hydrogels. The hydrogels contained less β-sheet crystalline and more amorphous structures than conventional, high-MW (HMW) SF hydrogels. Because of the potential loosened SF molecular structures in the hydrogel networks, the LMW SF hydrogels showed enhanced biodegradation (i.e., shorter in vitro enzymatic biodegradation time and faster in vivo biodegradation rate) as well as a lower affinity for plasma proteins and fibroblasts, which are involved in postoperative adhesion formation. An antiadhesion test using a rat abdominal adhesion model demonstrated that the LMW SF hydrogel applied to the abraded cecum was almost completely degraded within two weeks postimplantation, with a significantly lower adhesion severity score than that in the untreated model rat group. Conversely, the HMW SF hydrogel remained between the cecum and abdominal wall, with the same adhesion severity as that of the untreated model rat group. Therefore, we concluded that the antiadhesion effects of SF hydrogels were induced by enhanced biodegradation. The results of this study indicate the potential of LMW SF hydrogels as absorbable adhesion barriers.

Double network hydrogel confined MXene/Liquid metal by dynamic hydrogen bond for high-performance wearable sensors

Double-network (DN) hydrogels, which integrate long-chain and short-chain molecular structures, exhibit significant potential in wearable sensors due to their exemplary mechanical properties. However, conventional hydrogels often suffer from poor conductivity and low sensitivity. In this study, we develop a novel DN hydrogel (comprising polyacrylamide/sodium alginate) that encapsulates MXene (Ti3C2Tx) and liquid metal (LM). This configuration leverages the conductive properties of two-dimensional MXene and zero-dimensional liquid metal embedded within the DN hydrogel networks. The Ti3C2Tx MXene sheets enhance the binding capacity with LM by serving as a conductive bridge, thereby improving interfacial interactions and reducing hysteresis. The resultant strain sensor, fabricated from this composite DN hydrogel, achieves high sensitivity (gauge factor up to 12.84), a broad detection range (0 %-1500 %), rapid response time (262 ms), and excellent repeatability and stability. We have integrated this strain sensor into wearable flexible devices, such as contact lenses, enabling real-time monitoring of human physiological pressures.

Hydrogel network formation triggers atypical hygroscopic behavior in atmospheric aerosols.

The phase state of atmospheric aerosol particles, dictated by composition, intermolecular interaction, size, and pH, profoundly impacts climate, human health, and air quality. Herein, the phase behavior of internally mixed sodium bitartrate (SBT) and ammonium sulfate (AS) aerosols with equal molar ratio was studied using microscopic imaging, confocal Raman and infrared spectroscopy. We observed atypical phase transition during hygrosopic cycles. On dehydration, micro-solids formed at relative humidity (RH) of 80.1 % without further efflorescence, namely limited efflorescence (LE). On hydration, droplets effloresced at 39.8 % RH and deliquesced at 68.8 % RH, referred as efflorescence on hydration (EH). Raman spectra show that Na2SO4 solids form during LE, while both Na2SO4 and (NH4)2SO4 solids form during EH. The phase transition of the SBT/AS (1:1) droplets is size-dependent, where smaller droplets are prone to "EH" while larger droplets are prone to typical efflorescence. Combining AIOMFAC-VISC viscosity predictions with scanning electron microscopy (SEM) images, we attribute the "LE" and "EH" phenomena to the formation of an ion-organic hydrogel network structure within droplets. pH and organic/inorganic mixing ratios can collaboratively affect the stability of hydrogel network by changing the organic/inorganic mixing ratios. Our study shows that gel network formation can cause atypical phase transition in atmospheric aerosols.

Design, Characterization, and Biocompatibility of Modular Biopolymer-Based Single- and Double-Cross-Linked Networks Hydrogels

Design, Characterization, and Biocompatibility of Modular Biopolymer-Based Single- and Double-Cross-Linked Networks Hydrogels

Muscle‐Inspired Robust Anisotropic Cellulose Conductive Hydrogel for Multidirectional Strain Sensors and Implantable Bioelectronics

AbstractIntegrating superior mechanical performance, anisotropic conductivity, and biocompatibility into conductive hydrogels as all‐in‐one human‐machine interaction device remains challenging. Herein, by mimicking the anisotropic structures of human muscles, a robust anisotropic conductive hydrogel is developed by initially aligning polyvinyl alcohol with polypyrrole decorated cellulose nanofibrils to form an anisotropically oriented polymer networks, followed by post‐crosslinking with tannic acid (TA). Introducing TA into hydrogel network permanently secures its hierarchically anisotropic structure through multiple hydrogen bonds, thus endowing the hydrogel with exceptional mechanical properties (tensile strength of 11.41 MPa, toughness of 12.44 MJ m−3), anisotropic adhesive property, and direction‐dependent conductivity. With these attributes, a hydrogel strain sensor with excellent multidirectional sensitivity is developed, enabling stable monitoring of multi‐degrees of freedom joint movements in the human body and facilitating the control of a multiaxial virtual robot manipulator. Moreover, the in vitro/vivo tests demonstrate exceptional biocompatibility and anti‐biofouling properties of the as‐prepared hydrogel sensor, maintaining stable electronic response signals for over 14 days after successful implantation into the Achilles tendon of mice. Overall, this study presents a promising approach for designing conductive hydrogels with superior mechanical properties and anisotropic functionality for emerging applications in both in vitro and in vivo human‐machine interface materials.

Dynamic Water Microskin Induced by Photothermally Responsive Interpenetrating Hydrogel Networks for High‐Performance Light‐Tracking Water Evaporation

AbstractSolar‐driven interfacial water evaporation is attracting increasing attention as a promising environmentally‐friendly solution to freshwater scarcity. It has been proven that a thin water layer on photothermal materials can prevent solar energy from invalidly heating the excess water to enhance the evaporation rate. However, the current water layers are usually formed on inelastic materials via confined capillarity, which are static and uncontrollable. Herein, we propose a flexible hydrogel‐based photothermal conversion material with thermal responsiveness by facile frontal polymerization, which can generate a unique dynamic water microskin (DWMS) during the solar evaporation process. The copolymerized hydrogel, introduced by the second polymeric poly(vinyl alcohol) network and thermally responsive poly(N‐isopropylacrylamide) (PNIPAM), exhibits reinforced mechanical strength and photothermally triggers reversible shrinking/swelling cycles that enable a thin water layer (≈32 µm) to balance the feedwater supply and photothermic energy input dynamically. As a result, a stable superior vaporization rate of 8.7 kg m−2 h−1 is achieved based on a cylindrical hydrogel with 6 cm height under 1 sun. Moreover, the simultaneous responsive bending allows efficient omnidirectional solar evaporation by light‐tracking to ensure maximum perpendicular solar absorption, which provides an alternative strategy for durable high‐efficiency solar evaporators for effective thermal management and solar utilization.

In Situ Forming Hydrogel Reinforced with Antibiotic-Loaded Mesoporous Silica Nanoparticles for the Treatment of Bacterial Keratitis.

Bacterial keratitis (BK) is a serious ocular infection that can lead to vision impairment or blindness if not treated promptly. Herein, we report the development of a versatile composite hydrogel consisting of silk fibroin and sodium alginate, reinforced by antibiotic-loaded mesoporous silica nanoparticles (MSNs) for the treatment of BK. The drug delivery system is constructed by incorporating vancomycin- and ceftazidime-loaded MSNs into the hydrogel network. The synthesized MSNs were found to be spherical in shape with an average size of about 95nm. The loading capacities of both drugs were approximately 45% and 43%, for vancomycin and ceftazidime respectively. Moreover, the formulation exhibited a sustained release profile, with 92% of vancomycin and 90% of ceftazidime released over a 24h period. The cytocompatibility of the drug carrier was also confirmed by MTT assay results. In addition, we performed molecular dynamics (MD) simulations to better reflect the drug-drug and drug-MSN interactions. The results obtained from RMSD, number of contacts, and MSD analyses perfectly corroborated the experimental findings. In brief, the designed drug-MSN@hydrogel could mark an intriguing new chapter in the treatment of BK.

Reprocessible, Reusable, and Self-Healing Polymeric Adsorbent for Removing Perfluorinated Pollutants

Here, we report a reprocessible, reusable, self-healing, and form-switching polymeric adsorbent for remediating fluorinated pollutants in water. The copolymer hydrogel is designed to contain fluorophilic segments and cationic segments to induce strong binding with perfluorinated pollutants. The sorption performance reveals rapid and quantitative removal of these pollutants, driven by the synergistic effect of fluorophilic and electrostatic interaction. Importantly, a disulfide-containing dynamic crosslinker plays a crucial role in imparting multifunctionality. This enables self-healing by the restoration of crosslinks at the cut surfaces by disulfide exchange reactions and allows for the repeated use of the adsorbent via multiple adsorption–desorption cycles. Furthermore, the adsorbent is reprocessible by cleaving the crosslinks to afford linear copolymers, which can be repolymerized into a hydrogel network on demand. Also, form-switching capability is showcased through the aqueous self-assembly of linear copolymers into a fluorinated micelle, serving as another form of adsorbent for pollutant removal.

A Facile Strategy for Preparing Flexible and Porous Hydrogel-Based Scaffolds from Silk Sericin/Wool Keratin by In Situ Bubble-Forming for Muscle Tissue Engineering Applications.

In the present study, it is aimed to fabricate a novel silk sericin (SS)/wool keratin (WK) hydrogel-based scaffolds using an in situ bubble-forming strategy containing an N-(3-dimethylaminopropyl)-N'-ethylcarbodiimide hydrochloride (EDC) and N-hydroxysuccinimide (NHS) coupling reaction. During the rapid gelation process, CO2 bubbles are released by activating the carboxyl groups in sericin with EDC and NHS, entrapped within the gel, creating a porous cross-linked structure. With this approach, five different hydrogels (S2K1, S4K2, S2K4, S6K3, and S3K6) are constructed to investigate the impact of varying sericin and keratin ratios. Analyses reveal that more sericin in the proteinaceous mixture reinforced the hydrogel network. Additionally, the hydrogels' pore size distribution, swelling ratio, wettability, and in vitro biodegradation rate, which are crucial for the applications of biomaterials, are evaluated. Moreover, biocompatibility and proangiogenic properties are analyzed using an in-ovo chorioallantoic membrane assay. The findings suggest that the S4K2 hydrogel exhibited the most promising characteristics, featuring an adequately flexible and highly porous structure. The results obtained by in vitro assessments demonstrate the potential of S4K2 hydrogel in muscle tissue engineering. However, further work is necessary to improve hydrogels with an aligned structure to meet the features that can fully replace muscle tissue for volumetric muscle loss regeneration.

PH-Responsive Alginate/Chitosan Gel Films: An Alternative for Removing Cadmium and Lead from Water.

Biosorption, a non-expensive and easy method for removing potentially toxic metal ions from water, has been the subject of extensive research. In this context, this study introduces a novel approach using sodium alginate and chitosan, versatile biopolymers that have shown excellent results as biosorbents. The challenge of maintaining high efficiencies and reuse is addressed by developing alginate/chitosan-based films. These films, prepared using solvent casting and crosslinking methods, form a hydrogel network. The alginate/chitosan-based films, obtained using the eco-friendly polyelectrolyte complex method, were characterized by FTIR, SEM, TGA, and DSC. The study of their swelling pH response, adsorption, and desorption behavior revealed promising results. The adsorption of Pb was significantly enhanced by the presence of both biopolymers (98%) in a shorter time (15 min) at pH = 6.5. The adsorption of both ions followed a pseudo-second-order kinetic and the Langmuir isotherm model. The desorption efficiencies for Cd and Pb were 98.8% and 77.6% after five adsorption/desorption cycles, respectively. In conclusion, the alginate/chitosan-based films present a highly effective and novel approach for removing Cd and Pb from water, with a promising potential for reuse, demonstrating their strong potential in potentially toxic metal removal.

Photothermal-Induced Multimodal Antibacterial Dressing Comprising N-Halamine Hydrogel Loaded with Cow Dung Biochar for Infected Wound Healing.

Disposal of the cow dung pollutants arising from cattle farming threatens the environment and public safety in diverse ways. To date, researchers have worked on developing new pathways to control and manage cattle farming wastes, but most do not involve the reuse of these wastes. Herein, a cow dung biochar-modulated photothermal N-halamine hydrogel (i.e., PAN/CA/CoBC/pMAG-Cl) was designed for converting cow dung into biochar (CoBC), which was then coupled with a 3D interpenetrating hydrogel network to treat infected wounds. The PAN/CA/CoBC/pMAG-Cl hydrogel exhibited excellent synergistic antibacterial performance against 106 CFU·mL-1 Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) within 60 min. The bactericidal effect was multimodal, involving CoBC-based photothermal killing (i.e., temperature as high as 80.5 °C) after 808 nm near-infrared light irradiation for 10 min, contact killing through the strong oxidative characteristic of N-halamine (pMAG-Cl), and release killing via active halogens (i.e., Cl+) reinforced by the photothermal action of CoBC. The S. aureus-infected wound model in vivo demonstrated that the PAN/CA/CoBC/pMAG-Cl hydrogel worked as an ideal wound dressing, capable of resisting bacterial infection, accelerating the healing process, and promoting epithelial regeneration. This proposed strategy could indicate a new way for the disposal of cow dung pollutant and its reuse in antibacterial-associated applications.

Green synthesis of multifunctional responsive hydrogel embedded with silver, based on xanthan gum, N-isopropylacrylamide, vinyl imidazole, and Luffa cylindrica for wound healing

In this study, a pH- and temperature-responsive smart hydrogel was developed by utilizing Xanthan Gum (XG), N-Isopropylacrylamide (NIPAM), Vinyl Imidazole (VI), and Luffa cylindrical (LC). Semi-interpenetrating polymer networks (semi-IPNs) were created using free radical polymerization with N,N′-methylenebisacrylamide (MBA) as the cross-linker and ammonium persulfate (APS) as the initiator. Silver nanoparticles (AgNPs) were synthesized within semi-IPN hydrogel network structures to impart antibacterial properties. Malva sylvestris (MS) aqueous leaf extract was used as a reducing and stabilizing agent for the green synthesis of the AgNPs. The semi-IPN hydrogels exhibited pH- and temperature-responsive swelling behavior, which also enabled the controlled release of the drug. After 11 h, the cumulative release reached approximately 73% at pH 7.2 and 87% at pH 8.3. Additionally, the sustained release mechanism of the Trimethoprim drug was described using the Korsmeyer-Peppas model and was governed by Fickian diffusion. The drug-loaded semi-IPN@Ag nanocomposite hydrogel has demonstrated effective antibacterial activity against various Gram-negative and Gram-positive bacteria, indicating its promising potential as a wound dressing material for reducing infection risk.

Resolving dynamic and static characteristics of the fouling by alginate in membrane distillation via optical coherence tomography

In an effort to improve the efficiency of membrane distillation (MD) for recovering water from a high salinity feed, recent studies paid special attention to the effects of fouling by alginate, which is an anionic polysaccharide ubiquitously involved in marine sources. However, it is technically challenging to in-situ characterize the gel layer with a relatively low degree of optical visibility. Therefore, a particle-assisted strategy was proposed by this study to improve the characterization based on optical coherence tomography (OCT) and thereby resolve both the dynamic (i.e., relating to the spatiotemporal evolution) and static (i.e., relating to the morphological properties) characteristics for developing a gel layer in the MD process with an alginate-containing feed. When confirming the effectiveness of employing differently sized polystyrene microbeads as the tracer combined with alginate aggregates and the detector transferred into the network of hydrogel, all the characterization results reveal that the alginate aggregates could be deposited in a heterogeneous way to form a steady structure composed of a static layer (∼150 μm) and a dynamic layer (∼50 μm); ∼25% to ∼30% of the cross-sectional area could be dominated by submicron- and micron-sized fluid channels in the static layer. This study not only provides deeper insights into the fouling by alginate in MD, but also broadens the spectrum of OCT-based characterization.

Bacteria encapsulation into polyethylene glycol hydrogels using Michael-type addition reactions

AbstractHydrogel materials can be used to integrate bacteria cells into biohybrid systems. Here, we investigate the use of polyethylene glycol-based hydrogels that employ different Michael-type addition crosslinking chemistries, including thiol-acrylate, thiol-vinyl sulfone, and thiol-maleimide click reactions, for covalent hydrogel network formation and bacteria encapsulation. All crosslinking chemistries generated hydrogels that provided stable encapsulation and culture of Bacillus subtilis; however, significant differences in cell viability and cell morphology after encapsulation were identified. Thiol-acrylate hydrogels provided the highest cell viability and favored encapsulation of single cells, while thiol-maleimide hydrogels had the lowest cell viability and favored encapsulation of larger aggregates. These findings demonstrate the impact of crosslinking strategies for encapsulation of microorganisms into hydrogel networks and suggest that thiol-acrylate chemistries are favorable for many applications. Graphical abstract

Controlled stiffness and diffusivity of poly(ethylene glycol) hydrogel formed with cellulose-nanofiber framework

Hydrogels composed of polymer networks are widely used in industry and scientific research for high water retention and unique mechanical properties. Nevertheless, in ordinary hydrogel formation, the trade-off relationship between stiffness and mesh size remains a crucial consideration for practical applications. This study describes a facile approach to controlling hydrogel stiffness and mesh size by hybridizing poly(ethylene glycol) diacrylate (PEGDA) and methacrylated TEMPO-oxidized cellulose nanofibers (T-CNFMA). After disintegrating T-CNF by ultrasonication, T-CNFMA was synthesized resulting in a degree of substitution of 2.04 mmol/g. Incorporation of T-CNFMA in the PEGDA network allowed for independent control of hydrogel stiffness and mesh size by reinforcing the whole hydrogel network as a framework. Consequently, the swelling ratio and shear modulus could be manipulated by controlling the PEGDA/T-CNFMA ratio. Structural analyses revealed that an increase in the T-CNFMA content in the presence of a low amount of PEGDA resulted in a large mesh size with a constant stiffness. The diffusivity test was also consistent with the properties of the hydrogels. This result indicates that the incorporation of T-CNF in hydrogel network is useful to control the physical property of the hydrogel, especially for varying mesh size, regardless of stiffness alteration.

Simultaneous processing of both handheld biomixing and biowriting of kombucha cultured pre-crosslinked nanocellulose bioink for regeneration of irregular and multi-layered tissue defects

The nanocellulosic pellicle derived from the symbiotic culture of bacteria and yeast (Kombucha SCOBY) is an important biomaterial for 3D bioprinting in tissue engineering. However, this nanocellulosic hydrogel has a highly entangled gel network. This needs to be partially modified to improve its processability and extrusion ability for its applications in the 3D bioprinting area. To control its mechanical and biological properties for direct 3D bioprinting applications, uniform reinforcement of nanocellulose-interacting polymers and nanoparticles in such a prefabricated gel network is essential. In this study, the hydrogel network is partially hydrolyzed with organic acid and subsequently transformed into a 3D bioprintable polyelectrolyte complex with chitosan and kaolin nanoparticles without any chemical crosslinker using a handheld 3D bioprinter. This handheld bioprinter ensures homogeneity in both biomixing and bioprinting of chitosan and kaolin within the modified nanocellulose network for multi-layered bioprinted scaffolds through an extensional shear mechanism. The biomixing simulation, mechanical (static, dynamic, and cyclic), 3D bioprinting, and cellular studies confirm the homogeneous biomixing of kaolin nanoparticles and live cells in this nanocellulose-chitosan polyelectrolyte hydrogel. The combination of SCOBY-derived nanocellulose-chitosan bioink with kaolin nanoparticles and a screw-driven handheld extrusion bioprinter demonstrates a promising platform for layer-by-layer regeneration of complex tissues with homogeneous cell/particle distribution with high cell viability.

Preparation, Swelling, and Drug Release Studies of Chitosan-based Hydrogels for Controlled Delivery of Buspirone Hydrochloride.

Buspirone is used for the management of depression and anxiety disorders. Due to its short half-life and low bioavailability, it requires multiple daily doses and is associated with some side effects. This study aimed to develop chitosan-based hydrogels as drug-controlled release carriers. The objective of this study is to prepare chitosan-based hydrogels as controlled release carriers in order to overcome the side effects of buspirone HCl and improve patients' compliance and their life quality. Polymer chitosan was polymerized with two monomers, acrylic acid and itaconic acid, to synthesize pH-sensitive hydrogel. The Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) analysis were performed to confirm the structure formation and thermal stability. Water penetration capability and loading of the drug were performed by porosity and drug loading studies. The swelling and dissolution tests were performed to analyze the pH-sensitive nature of the developed hydrogels. FTIR, TGA, and DSC demonstrated that the chitosan-based hydrogels were successfully prepared. An increase in water penetration and drug loading into the hydrogel network was seen with the high incorporation of chitosan, acrylic acid, and itaconic acid. The swelling and dissolution studies revealed that prepared hydrogel offered the greatest swelling and drug release at a high pH of 7.4. The swelling and drug release from the hydrogel were affected by the concentrations of the incorporated contents. A controlled release of the drug was achieved by using chitosan-based hydrogel as a delivery carrier compared to commercial tablets of buspirone. The results showed that the developed chitosan-based hydrogel can be considered one of the most suitable drug carrier systems for the controlled delivery of buspirone.

Intelligent microneedle patch based on functionalized alginate and chitosan for long-term self-regulated insulin delivery

Severely diabetic patients need insulin input to maintain the body's glycemic balance. However, traditional injection methods are often associated with poor adherence and an increased risk of hypoglycemia. Microneedle technology offers a promising solution by minimizing pain and trauma during insulin administration. Nonetheless, achieving prolonged glycemic control by microneedle with high insulin loading remains a significant challenge. Herein, we introduce an innovative microneedle patch that draws inspiration from the elegant light-induced blooming of water lily petals. The patch features a glucose-responsive hydrogel network crafted from two modified polysaccharide polymers, which enables the delivery of long-acting insulin without depending on glucose oxidase. By incorporating phenylboronic acid-modified sodium alginate, quaternary ammonium chitosan, and polyvinyl alcohol into a hydrogel matrix, we have created a microneedle system that harbors dynamic borate ester linkages and electrostatic attractions, resulting in heightened sensitivity to blood glucose levels. The electrostatic interaction acts as a relatively stable crosslinking point, balancing the dynamic reproducibility response based on the borate ester bond. This self-adaptive hydrogel can regulate insulin-controlled release by responding to changes in glucose concentration. Herein, we achieved massive insulin loading (20 IU) with long lasting glycaemic control (48 h) in a single treatment of diabetic SD rats.

Metal welding-inspired phase change self-healing strategy applied to high-modulus hydrogel composites

The self-healing efficiencies of polymers are inversely proportional to their modulus, as the recovery of the polymer network heavily relies on the mobility of polymer chains. Therefore, reinvigorated by the metal welding, we have developed S-PAM-SA-x supercooling hydrogels, consisting of polyacrylamide hydrogel networks and inorganic CH3COONa·3H2O phase change materials. Subsequently, rigid self-healing H-PAM-SA-x composites were achieved via self-actuated crystallization-related phase change from the supersaturated hydrogels, resulting in a significant enhancement in mechanical properties. Notably, the Young’s modulus experienced an astonishing increase from 0.07 to 387.1 MPa. The H-PAM-SA-130 % composites demonstrated satisfactory self-healing performance based on the phase change of melting and crystallization, as the dominant mechanical carrier was found to be the crystal lattice rather than the PAM network. Leveraging the reversible nature of melting and crystallization, the same position can undergo multiple healing cycles without compromising self-healing efficiencies. Moreover, this distinctive dynamic phase change process significantly expands the range of functional applications, encompassing self-healing, adhesion, and patterns’ replication among others.