Physical Crosslinking Research Articles

A bacterial cellulose/polyvinyl alcohol/nitro graphene oxide double layer network hydrogel efficiency antibacterial and promotes wound healing

In this study, graphene oxide (GO) was chemically modified utilizing concentrated nitric acid to produce a nitrated graphene oxide derivative (NGO) with enhanced oxidation level, improved dispersibility, and increased antibacterial activity. A double-layer composite hydrogel material (BC/PVA/NGO) with a core-shell structure was fabricated by utilizing bacterial cellulose (BC) and polyvinyl alcohol (PVA) binary composite hydrogel scaffold as the inner network template, and hydrophilic polymer (PVA) loaded with antibacterial material (NGO) as the outer network. The fabrication process involved physical crosslinking based on repeated freezing and thawing. The resulting BC/PVA/NGO hydrogel exhibited a porous structure, favorable mechanical properties, antibacterial efficacy, and biocompatibility. Subsequently, the performance of BC/PVA/NGO hydrogel in promoting wound healing was evaluated using a mouse skin injury model. The findings demonstrated that the BC/PVA/NGO hydrogel treatment group facilitated improved wound healing in the mouse skin injury model compared to the control group and the BC/PVA group. This enhanced wound healing capability was attributed primarily to the excellent antibacterial and tissue repair properties of the BC/PVA/NGO hydrogel.

Anisotropic foams derived from textile-based cellulose nanocrystals and xanthan gum

The upcycling of discarded garments can help to mitigate the environmental impact of the textile industry. Here, we fabricated hybrid anisotropic foams having cellulose nanocrystals (CNCs), which were isolated from discarded cotton textiles and had varied surface chemistries as structural components, in combination with xanthan gum (XG) as a physical crosslinker of the dispersion used for foam preparation. All CNCs had crystallinity indices above 85 %, zeta potential values below −40 mV at 1 mM NaCl, and true densities ranging from 1.61 to 1.67 g·cm−3. Quartz crystal microbalance with dissipation (QCM-D) measurements indicated weak interactions between CNC and XG, while rheology measurements showed that highly charged CNCs caused the XG chains to change from an extended to a helicoidal conformation, resulting in changes the in viscoelastic properties of the dispersions.The inclusion of XG significantly enhanced the compression mechanical properties of the freeze-casted foams without compromising their thermal properties, anisotropy, or degree of alignment. CNC-XG foams maintained structural integrity even after exposure to high humidity (91 %) and temperatures (100 °C) and displayed very low radial thermal conductivities. This research provides a viable avenue for upcycling cotton-based clothing waste into high-performance materials.

Simultaneously improved H+ conductivity and H+/V4+ selectivity for all vanadium flow battery by ZIF-8 induced physical cross-linking

One of the major challenges in all vanadium redox flow battery (VRFB) is the trade-off between proton conductivity and vanadium ion cross-mixing. Here, we simultaneously enhanced proton conductivity and sharply reduced the vanadium crossover by introducing ZIF-8 into a sulfonated polyimide (6FTMA-100) to prepared a high performance VRFB membrane. Compared with the pristine membrane, the proton conductivity increased from 34.6 to 47.4 mS cm−1, and the vanadium ion permeation rates decreased from 3.56 × 10−7 to 0.82–1.88 × 10−7 cm2 min−1 with different ZIF-8 doping concentrations. The ZIF-8 doped membranes also showed increased viscosity, reduced membrane swelling ratio and increased Young's modulus. We propose this is due to the strong hydrogen bonding (−106.68 Kcal/mol) between the N in imidazole group and H in -SO3H. Battery performance confirmed that the optimized MMM-2 (2 % ZIF-8 loading) displayed the energy efficiency of 80 % at 160 mA cm−2 that much higher than its pristine 6FTMA-100, N117, and most of the reported sulfonated polyimides. This idea of creating physical crosslinked network provided an efficient way for achieving highly efficient VRFB membranes.

Ionic-physical–chemical triple cross-linked all-biomass-based aerogel for thermal insulation applications

Aerogels, as a unique porous material, are expected to be used as insulation materials to solve the global environmental and energy crisis. Using chitosan, citric acid, pectin and phytic acid as raw materials, an all-biomass-based aerogel with high modulus was prepared by the triple strategy of ionic, physical and chemical cross-linking through directional freezing technique. Based on this three-dimensional network, the aerogel exhibited excellent compressive modulus (24.89 ± 1.76 MPa) over a wide temperature range and thermal insulation properties. In the presence of chitosan, citric acid and phytic acid, the aerogel obtained excellent fire safety (LOI value up to 31.2%) and antibacterial properties (antibacterial activity against Staphylococcus aureus and Escherichia coli reached 81.98% and 67.43%). In addition, the modified aerogel exhibited excellent hydrophobicity (hydrophobic angle of 146°) and oil–water separation properties. More importantly, the aerogel exhibited a biodegradation rate of up to 40.31% for 35 days due to its all-biomass nature. This work provides a green and sustainable strategy for the production of highly environmentally friendly thermal insulation materials with high strength, flame retardant, antibacterial and hydrophobic properties.

Quaternary Ammonium Assisted Synthesis of Melanin-like Poly(l-DOPA) Nanoparticles with a Boosted Photothermal Effect.

Poly(levodopa) nanoparticles (P(l-DOPA) NPs) are another kind of melanin mimetic besides well-established polydopamine nanoparticles (PDA NPs). Due to the presence of carboxyl groups, the oxidative polymerization of l-DOPA to obtain particles was not as efficient as that of dopamine. Several established methods toward P(l-DOPA) NP fabrication do not combine convenience, morphological regularity, size controllability, low cost, and adaptability to metal-free application scenarios. In this work, P(l-DOPA) NPs were successfully prepared in hot water with the assistant of organic quaternary ammonium, due to the extra physical cross-linking mediated by cations. The employed physical interactions could also be affected by quaternary ammonium structure (i.e., number of cation heads, length of alkyl chain) to achieve different polymerization acceleration effects. The obtained P(l-DOPA) NPs retained superior photothermal properties and outperformed PDA-based melanin materials. Furthermore, P(l-DOPA) NPs were used in photothermal tumor therapy and showed better efficacy. This study offers new insights into the synthesis of melanin-like materials, as well as new understanding of the interaction between quaternary ammonium and bioinspired polyphenolic materials.

The study of double-network carboxymethyl chitosan/sodium alginate based cryogels for rapid hemostasis in noncompressible hemorrhage

Developing an injectable hemostatic dressing with shape recovery and high blood absorption ratio for rapid hemostasis in noncompressible hemorrhage maintains a critical clinical challenge. Here, double-network cryogels based on carboxymethyl chitosan, sodium alginate, and methacrylated sodium alginate were prepared by covalent crosslinking and physical crosslinking, and named carboxymethyl chitosan/methacrylated sodium alginate (CM) cryogels. Covalent crosslinking was achieved by methacrylated sodium alginate in the freeze casting process, while physical crosslinking was realized by electrostatic interaction between the amino group of carboxymethyl chitosan and the carboxyl group of sodium alginate. CM cryogels exhibited large water swelling ratios (8167 ± 1062 %), fast blood absorption speed (2974 ± 669 % in 15 s), excellent compressive strength (over 160 kPa for CM100) and shape recovery performance. Compared with gauze and commercial gelatin sponge, better hemostatic capacities were demonstrated for CM cryogel with the minimum blood loss of 40.0 ± 8.9 mg and the lowest hemostasis time of 5.0 ± 2.0 s at hemostasis of rat liver. Made of natural polysaccharides with biocompatibility, hemocompatibility, and cytocompatibility, the CM cryogels exhibit shape recovery and high blood absorption rate, making them promising to be used as an injectable hemostatic dressing for rapid hemostasis in noncompressible hemorrhage.

A TLR4-Targeting Bioactive Peptide Hydrogel to Regulate Immune-Microenvironment for Diabetic Wound Repair.

Persistent inflammation and disrupted immunoregulation are critical factors in impeding diabetic wound healing. While immunoregulatory hydrogel dressings hold significant promise for clinical applications in diabetic wound healing, the current application often demands intricate interventions and high-cost treatments involving cytokines and cell therapies. The development of single component immunoregulatory hydrogels remains a complex challenge. To address this issue, an active peptide hydrogel with immunoregulatory properties targeting the TLR4/NF-kB pathway, aiming to promote rapid diabetic wound healing, is engineered. The hydrogel sequence comprises naphthalene derivative, phenylalanine, and glycine to modulate hydrophilic/hydrophobic characteristics. The amino group on arginine contributes to tissue adhesion and regulation of intermolecular forces, ultimately yielding stable gels. The results underscore the formation of the peptide hydrogel (NFA) via the physical crosslinking of self-assembled nanofibers in water, thereby affording both excellent injectability and tissue adhesion. Notably, NFA demonstrates significant potential in promoting wound healing in a mouse model with full-thickness wounds by regulating macrophage responses in the inflammatory microenvironment through the TLR4/NF-kB pathway.

Evaluation of the effect of the incorporation of poly(lactic acid) and maleic anhydride in the thermoshrinkage of films from thermoplastic starch

AbstractStudies on the property of shape memory in thermoplastic starch (TPS) have shown good results, making such starch a suitable candidate for use in shrink packaging. It is however necessary to evaluate blending it with other bioplastics that would improve its properties while maintaining heat shrinkage. This article thus shows the evaluation of the incorporation of different concentrations of polylactic acid (PLA) and maleic anhydride (MA) as coupling agent and their effect on shrinkage and the changes in structure of the films obtained by blown film extrusion. In most of the blends, the incorporation of PLA and MA was found to favor film shrinkage, obtaining values of up to 55% due to the fact that the interaction between TPS and PLA increased with the incorporation of MA. This was corroborated by the % of MA grafted, thermogravimetric analysis (TGA), rheological and structural tests. This allowed generating a greater molecular orientation of the films, thereby obtaining greater shrinkage. It was determined that the incorporation of PLA and % MA grafted generated good shrinkage results due to the physical and chemical crosslinking achieved in the processing of the blends in the presence of MA, enhancing their application as packaging.

Recent advances in polymers, preparation techniques, applications and future perspectives of hydrogels

Drug delivery via hydrogel is one of the most effective methods. Hydrogels have been described as polymeric water-swollen materials and retain water in distinctive three-dimensional complex. These are classified as pH sensitive hydrogels, temperature sensitive hydrogels, homo-polymer hydrogels, co-polymer hydrogels and Interpenetrating Network (IP-N) hydrogel. Hydrogels can be prepared via various techniques, including physical crosslinking, chemical crosslinking, free radical polymerization, photo-initiator’s and hydrogen bonding. Various polymers in manufacturing includes pectin, chitosan, cyclodextrin and carrageenan, etc. This review aims to describes hydrogels for drug delivery, classifications, preparation techniques, various polymers in hydrogel preparation and highlights novel applications of hydrogels in medicine.

Shape memory polyimide/carbon nanotube composite aerogels with physical and chemical crosslinking architectures for thermal insulating applications

The development of lightweight smart materials with exceptional shape memory and thermal insulation properties is highly important in the aerospace industry. The reported shape memory polymer aerogels (SMPAs) are restricted to harsh environments because of their poor high-temperature resistance and large volume shrinkage at elevated temperatures. Herein, shape memory polyimide (PI) composite aerogels with superior thermal insulation were fabricated by combining molecularly designed PI chains with amino-functionalized carbon nanotubes (NH2-CNTs) through freezing gelation and subsequent thermal imidization. Because shape memory behavior was thermally triggered, the thermal conductivity associated with the shape memory mechanisms of the aerogels was comprehensively explored. The presence of CNTs promoted heat transfer in the aerogel skeleton, facilitating the shape recovery response. Benefiting from chemical-crosslinked and physical-crosslinked structures, the fabricated PI composite aerogels demonstrated desirable thermo-mechanical properties, exceptional shape memory and superior thermal insulation performance. This study may provide guidelines for designing shape memory PI composite aerogels for harsh environment applications in aerospace engineering.

Nanocomposite Methacrylated Silk Fibroin-Based Scaffolds for Bone Tissue Engineering.

The treatment of bone defects is a clinical challenge. Bone tissue engineering is gaining interest as an alternative to current treatments, with the development of 3D porous structures (scaffolds) helpful in promoting bone regeneration by ensuring temporary functional support. In this work, methacrylated silk fibroin (SilMA) sponges were investigated as scaffolds for bone tissue engineering by exploiting the combination of physical (induced by NaCl salt during particulate leaching) and chemical crosslinking (induced by UV-light exposure) techniques. A biomimetic approach was adopted to better simulate the extracellular matrix of the bone by introducing either natural (mussel shell-derived) or synthetic-origin hydroxyapatite nanoparticles into the SilMA sponges. The obtained materials were characterized in terms of pore size, water absorption capability and mechanical properties to understand both the effect of the inclusion of the two different types of nanoparticles and the effect of the photocrosslinking. Moreover, the SilMA sponges were tested for their bioactivity and suitability for bone tissue engineering purposes by using osteosarcoma cells, studying their metabolism by an AlamarBlue assay and their morphology by scanning electron microscopy. Results indicate that photocrosslinking helps in obtaining more regular structures with bimodal pore size distributions and in enhancing the stability of the constructs in water. Moreover, the addition of naturally derived hydroxyapatite was observed to be more effective at activating osteosarcoma cell metabolism than synthetic hydroxyapatite, showing a statistically significant difference in the AlamarBlue measurement on day 7 after seeding. The methacrylated silk fibroin/hydroxyapatite nanocomposite sponges developed in this work were found to be promising tools for targeting bone regeneration with a sustainable approach.

Cucurbit[8]uril Mediated Supramolecular and Photocrosslinked Interpenetrating Network Hydrogel Matrices for 3D-Bioprinting.

Printing of biologically functional constructs is significant for applications in tissue engineering and regenerative medicine. Designing bioinks remains remarkably challenging due to the multifaceted requirements in terms of the physical, chemical, and biochemical properties of the three-dimensional matrix, such as cytocompatibility, printability, and shape fidelity. In order to promote matrix and materials stiffness, while not sacrificing stress relaxation mechanisms which support cell spreading, migration, and differentiation, this work reports an interpenetrating network (IPN) bioink design. The approach makes use of a chemically defined network, combining physical and chemical crosslinking units with a tunable composition and network density, as well as spatiotemporal control over post-assembly material stiffening. To this end, star-shaped poly(ethylene glycol)s functionalized with Phe-Gly-Gly tripeptide or photoactive stilbazolium are synthesized, and used to prepare three-dimensional networks with cucurbit[8]uril (CB[8]) through supramolecular host-guest complexation. The hydrogel obtained shows fast relaxation and thus supports the proliferation and differentiation of cells. Upon irradiation, the mechanical properties of the hydrogel can be rapidly adapted via selective photochemical dimerization of stilbazolium within CB[8], leading to IPNs with increased form stability while retaining the dynamic nature of the hydrogels. This modular approach opens new design opportunities for extrudable and cell-friendly dynamic biomaterials for applications in 3D-bioprinting.

Preparation and evaluation of chitosan/MCM-41-based spongy hydrogels loaded with tea tree oil

In this study, chitosan, polyvinyl alcohol, gelatin, MCM-41 and tea tree oil (TTO) were used as raw materials. MCM-41-based spongy hydrogels loaded with TTO were synthesized by physical cross-linking method. The TTO was first adsorbed into MCM-41 s. Then different contents of MCM-41 s were added to the hydrogel, which affected the properties of the hydrogel. The structure of hydrogels was analyzed by scanning electron microscopy (SEM) and attenuated total internal reflectance Fourier transform infrared spectroscopy (ATR-FTIR). The mechanical properties of hydrogels were determined by swelling, degradation and ductility evaluation. The antibacterial effect and biocompatibility were determined by in vitro antibacterial and cytotoxicity examinations. In this study, the mechanical property of the hydrogels was enhanced with the increasing content of MCM-41 s. The hydrogels exhibited an excellent antibacterial effect attributed to the synergistic interaction between TTO and chitosan. Furthermore, the hydrogels showed superior biocompatibility property. In conclusion, the hydrogels prepared in this study have great potential for expanding their applications in the bacteriostatic field.

Facilitating safe and sustained submucosal lift through an endoscopically injectable shear-thinning carboxymethyl starch sodium hydrogel

Traditional submucosal filling materials frequently show insufficient lifting height and duration during clinical procedures. Here, the anionic polysaccharide polymer sodium carboxymethyl starch and cationic Laponite to prepare a hydrogel with excellent shear-thinning ability through physical cross-linking, so that it can achieve continuous improvement of the mucosal cushion through endoscopic injection. The results showed that the hydrogel (56.54 kPa) had a lower injection pressure compared to MucoUp (68.56 kPa). The height of submucosal lifting height produced by hydrogel was higher than MucoUp, and the height maintenance ability after 2 h was 3.20 times that of MucoUp. At the same time, the hydrogel also showed satisfactory degradability and biosafety, completely degrading within 200 h. The hemolysis rate is as low as 0.76 %, and the cell survival rate > 80 %. Subcutaneous implantation experiments confirmed that the hydrogel showed no obvious systemic toxicity. Animal experiments clearly demonstrated the in vivo feasibility of using hydrogels for submucosal uplift. Furthermore, successful endoscopic submucosal dissection was executed on a live pig stomach, affirming the capacity of hydrogel to safely and effectively facilitate submucosal dissection and mitigate adverse events, such as bleeding. These results indicate that shear-thinning hydrogels have a wide range applications as submucosal injection materials.

Camellia meal-based adhesive with synergistic crosslinking of physical and chemical interaction for preparing aldehyde-free, anti-mildew, water-resistant wood-based composites

Wood adhesives containing toxic aldehyde-based adhesives play a vital role in the performance of wood-based panels, while the mechanical properties and water and mildew resistance of aldehyde-free adhesives are lacking. In this study, a high-strength aldehyde-free adhesive was constructed via a combination of physical and chemical crosslinks. Inexpensive alum was used to ensure a high degree of crosslinking and to increase the crystallinity. Metal ions in alum opened the protein helix, exposed the active groups, increased the number of hydrogen bonds, and ultimately improved the internal physical crosslinking ability of the adhesive. The compound formed by the Schiff base reaction formed coordination bonds with metal ions, thus forming a covalently-crosslinked network. The high-strength polymer produced in this study contained multiple physical and covalent crosslinks, resulting in significantly improved mechanical properties of the adhesive. Its water-resistant adhesive strength reached 1.96 MPa, which was 180.2% higher than that of ordinary phytogenic protein adhesive (0.69 MPa), and it can still reach 1.28 MPa after hot water circulation soaking experiment. The adhesive also possessed antifungal properties and flame-retardant capabilities, achieving a V-1 rating in the UL-94 test. This strategy expanded the application of phytogenic protein adhesives in environmentally friendly wood composite materials by replacing synthetic resins that released formaldehyde and provided an economical and feasible industrial scale production method for the preparation of high strength, water, and mildew resistant, flame retardant indoor and outdoor wood-based panels.

From ionic clusters dynamics to network constraints in ionic polymer solutions.

Physical networks formed by ionizable polymers with ionic clusters as crosslinks are controlled by coupled dynamics that transcend from ionic clusters through chain motion to macroscopic response. Here, the coupled dynamics, across length scales, from the ionic clusters to the networks in toluene swollen polystyrene sulfonate networks, were directly correlated, as the electrostatic environment of the physical crosslinks was altered. The multiscale insight is attained by coupling neutron spin echo measurements with molecular dynamics simulations, carried out to times typical of relaxation of polymers in solutions. The experimental dynamic structure factor is in outstanding agreement with the one calculated from computer simulations, as the networks are perturbed by elevating the temperature and changing the electrostatic environment. In toluene, the long-lived clusters remain stable over hundreds of ns across a broad temperature range, while the polymer network remains dynamic. Though the size of the clusters changes as the dielectric constant of the solvent is modified through the addition of ethanol, they remain stable but morph, enhancing the polymer chain dynamics.

Mucus-Mimicking Mucin-Based Hydrogels by Tandem Chemical and Physical Crosslinking.

Mucosal tissues represent a major interface between the body and the external environment and are covered by a highly hydrated mucins gel called mucus. Mucus lubricates, protects and modulates the moisture levels of the tissue and is capitalized in transmucosal drug delivery. Pharmaceutical researchers often use freshly excised animal mucosal membranes to assess mucoadhesion and muco-penetration of pharmaceutical formulations which may struggle with limited accessibility, reproducibility, and ethical questions. Aiming to develop a platform for the rationale study of the interaction of drugs and delivery systems with mucosal tissues, in this work mucus-mimicking mucin-based hydrogels are synthesized by the tandem chemical and physical crosslinking of mucin aqueous solutions. Chemical crosslinking is achieved with glutaraldehyde (0.3% and 0.75% w/v), while physical crosslinking by one or two freeze-thawing cycles. Hydrogels after one freeze-thawing cycle show water content of 97.6-98.1%, density of 0.0529-0.0648gcm⁻3, and storage and loss moduli of ≈40-60 and ≈3-5Pa, respectively, that resemble the properties of native gastrointestinal mucus. The mechanical stability of the hydrogels increases over the number of freeze-thawing cycles. Overall results highlight the potential of this simple, reproducible, and scalable method to produce artificial mucus-mimicking hydrogels for different applications in pharmaceutical research.

Physical studies of chitosan/PEG loaded Fe2O3 nanoparticles microbeads as a based biodegradable material for radiation shielding

This work reports two different strategies for the formation of hybrid microbeads using chitosan and polyethylene glycol (PEG) as based biodegradable materials for radiation shielding. An organic–inorganic hydrogel was prepared by ionotropic gelation. During the in-situ loading, incorporating magnetic nanoparticles Fe2O3 into the polymer matrix, magnetic nanostructures, were entrapped in the polymer matrix during the physical cross-linking of the polymer with the physical cross-linker (sodium triphosphate). However, in case of post-loading mechanism the loaded nanoparticles favor the precipitation on the surface of the formed beads. We use different characterization techniques for our systems such as scanning electron microscopy (SEM), x-ray, infrared spectroscopy (XRD), and X-ray radiation shielding application. The results demonstrate that by incorporating nanostructured magnetic particles into the polymer matrix, the surface morphology based on the two processes allow the magnetic nanoparticles to be embedded or form an outer shell and precipitated on the surface of polymer microbeads. The values of μ for the hydrogels loaded with Fe2O3 by in-situ process have the larger values of the linear coefficient however, in case of post-loading process the values dramatically decrease in compare with the in-situ ones at the same tube voltage. The presented work recommended as a good mentor for radiation shielding.

Chitosan-Oxidized Pullulan Hydrogels Loaded with Essential Clove Oil: Synthesis, Characterization, Antioxidant and Antimicrobial Properties.

Emulsion hydrogels are promising materials for encapsulating and stabilizing high amounts of hydrophobic essential oils in hydrophilic matrices. In this work, clove oil-loaded hydrogels (CS/OP-C) are synthesized by combining covalent and physical cross-linking approaches. First, clove oil (CO) was emulsified and stabilized in a chitosan (CS) solution, which was further hardened by Schiff base covalent cross-linking with oxidized pullulan (OP). Second, the hydrogels were subjected to freeze-thaw cycles and, as a result, the clove oil was stabilized in physically cross-linked polymeric walls. Moreover, due to cryogelation, the obtained hydrogels exhibited sponge-like porous interconnected morphology (160-250 µm). By varying the clove oil content in the starting emulsion and the degree of cross-linking, the hydrogels displayed a high water retention capacity (swelling ratios between 1300 and 2000%), excellent elastic properties with fast shape recovery (20 s) after 70% compression, and controlled in vitro clove oil release in simulated skin conditions for 360 h. Furthermore, the prepared clove oil-loaded hydrogels had a strong scavenging activity of 83% and antibacterial and antifungal properties, showing a bacteriostatic effect after 48 and 72 h against S. aureus and E. coli. Our results recommend the new clove oil-embedded emulsion hydrogels as promising future materials for application as wound dressings.

Synthesis and characterization of ureidopyrimidinone-functionalized polyurethane acrylates and their hybrid nanocomposites for UV coating applications

In this study, ureidopyrimidinone moieties (UPy), capable of physical crosslinking via quadruple hydrogen bonding, were successfully incorporated into UV-curable polyurethane acrylate prepolymers. First, a hydroxyl-terminated unsaturated ester monomer was synthesized and reacted with isophorone diisocyanate to create a hydroxyl-terminated UV-curable urethane oligomer (U–OH). Then, isocyanate-terminated building blocks (UPy moieties and an acrylate-based photosensitive monomer) were synthesized and used in various ratios to functionalize U–OH for the preparation of a series of UV-curable UPy-containing polyurethane acrylate (PUA) resins. The resulting products were structurally characterized using 1H NMR and FTIR spectroscopy. Furthermore, organic–inorganic hybrid nanocomposites were obtained by introducing silane coupling agents into PUA resins using the sol–gel process. A series of UV-curable UPy-containing PUA coatings and hybrid nanocomposites were prepared, and their synergistic effect on coating properties was investigated. The dynamic mechanical analysis revealed that the Tg of the samples increased with increasing UPy content, although the mechanical properties remained largely unaltered, as shown by the stress–strain test. The studies also demonstrated that the hybrid nanocomposites exhibited higher decomposition temperatures and better thermal stability compared to pure PUAs. All the coatings exhibited good transparency in the visible region. An optical microscope was used to investigate the self-healing property by scratching the plexiglass panels with a razor blade. Among the other samples, the coating with the highest percentage of UPy content exhibited the best self-healing ability after heat treatment at 90 °C for 10 min.Graphical abstract