This study provides an experimental basis for developing a new type of wound repair materials that integrate antioxidant, anti-infective, and mechanically adaptive properties, holding significant application potential in oxidative stress-related tissue repair fields.
Abstract
Given the urgent need to regulate oxidative stress microenvironments in chronic wound healing, hydrogel dressings that simultaneously integrate antioxidant, antibacterial, mechanically adaptive, and biocompatible properties are highly desirable. In this study, a natural polymer-based composite hydrogel dressing loaded with zinc-quercetin nanozyme (Zn-Q) was designed. The gel skeleton was constructed via a dual network of photocrosslinked methacrylated silk fibroin (SilMA) and mercaptolated hyaluronic acid (HA-SH) via thiol-ene click chemistry, with the catalase (CAT)-like Zn-Q nanozyme encapsulated in situ within the network, thereby achieving synergy between chemical crosslinking and dynamic metal-polyphenol coordination. Systematic characterization revealed that Zn-Q nanozyme adopted a stable octahedral coordination configuration, and its continuous porous structure exposed abundant catalytically active sites. The composite hydrogels exhibited a highly interconnected, three-dimensional (3D) porous morphology, with swelling ratios that increased significantly with Zn-Q nanozyme content (up to around 1082%). Rheological and mechanical tests demonstrated that although incorporating the nanozyme reduced the storage modulus, the reversible physical crosslinks formed via hydrogen bonding and coordination interactions endowed the material with excellent tensile toughness and energy-dissipation capacity, exhibiting typical Mullins softening behavior. Functional evaluation showed that Zn-Q nanozyme conferred superior free radical scavenging capability to the hydrogels and exerted dose-dependent inhibition against both Staphylococcus aureus and Escherichia coli. Furthermore, the hydrogels exhibited favorable adhesion to various wet organs and heterogeneous material surfaces, with hemolysis rates below 5% and cell viability exceeding 100% after 3 days of culturing with fibroblasts, confirming their excellent hemocompatibility and cytocompatibility. This study provides an experimental basis for developing a new type of wound repair materials that integrate antioxidant, anti-infective, and mechanically adaptive properties, holding significant application potential in oxidative stress-related tissue repair fields.
Stable hydrogel formation with favorable porous architecture, swelling behavior, thermal stability, and homogeneous distribution of nanovesicles was well established and exhibited excellent biocompatibility, hemocompatibility, and enhanced cell-material interactions.
Rizos Evangelos Bikiaris, Ioanna Koumentakou, A. Niti et al.· ACS Applied Bio Materials· 0 citations
Hemolysis assays and cytocompatibility evaluations confirmed the favorable hemocompatibility of the HTP hydrogels, which significantly promoted fibroblast proliferation and migration, indicating their substantial potential for wound healing applications.
Lei Nie, Xinran Li, Mengfei Feng et al.· International Journal of Bio...· 0 citations
Diabetic wounds remain difficult to treat due to bacterial resistance, a localized weakly acidic microenvironment, imbalanced oxidative stress, and poor dressing conformity. To address these challenges, this study developed an injectable pH-responsive nanocomposite hydrogel using phenylboronic acid-modified chitosan (PBCS), tannic acid (TA), and porphyrinic metal–organic framework PCN-224 nanoparticles, featuring with superior tissue adhesiveness, self-healing, and pH-responsiveness. The hydrogel was fabricated using PBCS as the matrix and TA as the cross-linker, establishing a dual-cross-linked network sustained by dynamic boronate ester bonds and multiple hydrogen bonds, into which the porphyrinic metal–organic framework (MOF) PCN-224 was subsequently loaded. This hydrogel precisely senses and exploits the endogenous weakly acidic microenvironment of the infected wound, triggering the dissociation of boronate ester bonds to achieve the on-demand release of TA, as well as the smart regulation of the network’s swelling behavior. The synchronously released polyphenol component, TA, imparts excellent antioxidant activity to scavenge excess free radicals and re-establish oxidative stress balance. Meanwhile, under 660 nm laser irradiation, PCN-224 generated reactive oxygen species and a mild photothermal effect, enabling combined photodynamic and photothermal antibacterial activity. Collectively, the PBCS-TA/PCN-224 nanocomposite hydrogel integrates pH-responsive behavior, antioxidant activity, and light-triggered antibacterial functionality, supporting its potential application in infected diabetic wounds.
Jia-Yun Wang, He-Rui Yan, Fang-Ying Li et al.· ACS Applied Nano Materials· 0 citations
Polyacrylic acid-based composites hold substantial promise for intelligent wound dressing applications, owing to their intrinsic hydrophilicity and pH responsiveness. Nevertheless, their clinical translation is hindered by insufficient mechanical properties and excessive adhesion, which are directly induced by high hydrophilicity. Herein, a dual-network Janus hydrogel based on polyacrylic acid (PAA) and sodium alginate (SA), denoted as tannic acid-iron nanoparticles@polyacrylic acid/sodium alginate (TA-Fe NPs@PS Janus), was rationally fabricated. This hydrogel incorporates self-assembled TA-Fe nanoparticles (TA-Fe NPs) with inherent antibacterial activity and magnetic responsiveness. Magnetic enrichment of nanoparticles at the bottom side of the hydrogel not only significantly enhances mechanical toughness via metal-phenolic network (MPN) but also renders the top and bottom layers with distinct intelligent responses to heterogeneous pH microenvironments, thus enabling effective antibiotic-free treatment of infected wounds. TA-Fe NPs@PS Janus integrates high mechanical toughness, sensing performance, and pH responsiveness, enabling monitoring of wound microenvironmental changes through combined responses to pH and ionic variations throughout the recovery process. The physicochemical, mechanical, and rheological properties of the hydrogel were systematically characterized, and in vitro antibacterial assessments were conducted. Results demonstrate that TA-Fe NPs significantly enhance hydrogel toughness: compared with the pristine PAA/SA hydrogel (PS), the composite hydrogel incorporating 0.3% (w/v) TA-Fe NPs exhibits a 1200% increase in tensile toughness (from 0.06 MJ m⁻³ to 0.78 MJ m⁻³). The hydrogel displays high sensitivity and undergoes reversible deformation and intelligent responsive behavior under cyclic pH changes. It not only exhibits high antibacterial efficacy but also demonstrates favorable cytocompatibility. Therefore, this study proposes a smart, stimuli-responsive multifunctional hydrogel dressing for treating chronic wound inflammation and monitoring the healing process, highlighting its potential for clinical applications. STATEMENT OF SIGNIFICANCE: Chronic infected wounds severely threaten human health, yet clinically viable smart wound dressings are lacking. Polyacrylic acid (PAA) hydrogels are attractive for wound management but suffer from poor mechanical toughness and over-adhesion. We fabricate a dual-network Janus hydrogel (TA-Fe NPs@PS Janus) incorporating PAA, sodium alginate and tannic acid-iron nanoparticles. Magnetically concentrated TA-Fe NPs form metal-phenolic networks, boosting toughness by 1044.2% and creating asymmetric pH responsiveness. This cytocompatible hydrogel achieves antibiotic-free antibacterial function and real-time infection monitoring via pH changes. It overcomes key drawbacks of PAA hydrogels, integrates diagnosis and therapy, and offers a translatable strategy for intelligent chronic wound dressings.
Qing-Che Pan, Xin-Wei Tao, Jianliang Li et al.· Acta Biomaterialia· 0 citations
Hydrogel dressings have emerged as versatile platforms for wound management. However, the clinical performance of the hydrogel remains limited by insufficient mechanical robustness at joints, where repetitive deformation can compromise structural integrity and delay healing. To address these challenges, a nanocomposite dressing (GD@Bet-NWs) was fabricated by integrating gelatin methacrylate anhydride-grafted with dopamine hydrochloride (GelMA-DA), oxidized Tremella fuciformis polysaccharide (OTFP), carboxymethyl chitosan (CMC), polyvinyl alcohol (PVA), and borax. The hydrogel matrix was further augmented by incorporating selenium-functionalized polydopamine-polypyrrole (Se@PDA-PPy) nanowires (NWs) and Betulin (Bet)- encapsulated Pluronic F127 micelles (BetF127). The incorporation of Se@PDA-PPy NWs endowed the hydrogel with robust mechanical strength, adhesion, and exceptional antibacterial (> 98%) and ROS/RNS-scavenging (> 98%) potential. Encapsulation of Bet into Pluronic F127 micelles significantly improved its aqueous solubility and stability while alleviating pharmacokinetic limitations. In a full-thickness wound model, GD@Bet-NWs promoted re-epithelialization and collagen deposition, achieving 99% wound closure within 14 days. Immunohistochemical and immunofluorescence analyses revealed reduced levels of inflammatory cytokines and increased M2 macrophage polarization. Gene expression profiling further demonstrated the upregulation of immunomodulatory and tissue-regenerative genes, along with the downregulation of pro-inflammatory pathways. Consequently, the GD@Bet-NWs hydrogel dressing holds significant potential as an advanced wound-healing platform.
Muhammad Shahid, Mujahid Niaz, Huma Ghazal et al.· Journal of Controlled Releas...· 0 citations
In recent years, hydrogels have emerged as viable candidates for soft conductors in wearable flexible electronics, due to their distinctive properties including high water content, excellent biocompatibility, and adjustable mechanical properties. However, the crystallization of H2O molecules within hydrogels at low temperatures leads to significant deterioration in their toughness and mechanical strength, severely restricting their practical applications in cold environments. Cellulose nanocrystals (CNCs), rod-like nanomaterials with high crystallinity extracted from natural cellulose, have attracted increasing attention due to their outstanding mechanical properties, biocompatibility, and environmental friendliness. In this study, hyaluronic acid (HA) was adsorbed onto the surface of CNCs via hydrogen bonding, forming CNCs@HA nanomaterials. And then zwitterion proline (ZP) and CNCs@HA were incorporated into an acrylic acid-based hydrogel system, resulting in the formation of a novel freeze-resistant and self-healing nanocomposite hydrogel PAA-CNCs@HA-ZP-Fe3+ (PCHZF). The excellent properties of PCHZF can be attributed to the strong hydrogen bonding network formed among water molecules, CNCs@HA, and ZP molecules. These intermolecular interactions effectively inhibit the crystallization of water and maintain the integrity of the hydrogel matrix at low temperatures. Its compressive strength reaches 2.2 MPa, with a remarkable self-healing efficiency of 88.2%, and it can even achieve reliable sensing performance at extremely low temperatures.
Xiaohui Liu, Shaoning Shi, Jiarui Liu et al.· Colloids and Surfaces B: Bio...· 0 citations
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