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•A natural hydrogel-elastomer hybrid featured as tough, tissue adhesive, and tissue regeneration promotive was developed.•The adhesive strength could be adjusted by changing the ...formulation of hydrogel.•The hybrids were demonstrated excellent biocompatibility both in vitro and in vivo.•In vivo study confirmed the hybrid could promote the healing of meniscus tear.
Hydrogel adhesives are gaining popularity in tissue engineering and regeneration medicine. However, unsatisfactory anti-tension properties of traditional hydrogels limit their practical uses, particularly in sports medicine, which usually requires robust mechanical properties. Here, we design a tissue adhesive patch based on a bioadhesive hydrogel (HAMA-GelNB) and a tough elastomer (PDMS) that can atraumatically and rapidly repair tissue injuries such as meniscus tears. The strong and sutureless sealing capabilities of the hybrids are demonstrated using ex vivo porcine skin and stomach models. In vitro cell studies and in vivo subcutaneous implantation models are used and demonstrated the biocompatibility of the material. Finally, the efficiency of the tissue adhesive patch is demonstrated using a rabbit meniscus tear model which is challenging in clinic. The results of macroscopic images and histological analysis revealed that the surface of cartilage in the material-treated group was slightly worn, but the untreated group developed progressive cartilage degeneration. These findings demonstrate that the hydrogel-elastomer composite tissue adhesive could be an alternative to sutures for tissue repair and is promising in translational medicine.
The skin is the largest organ of the human body. Skin injuries, especially full-thickness injuries, are a major treatment challenge in clinical practice. Therefore, wound dressing materials with ...therapeutic effects have great practical significance in healthcare. This study used photocrosslinkable gelatin methacryloyl (GelMA) and sulfhydrylated chitosan (CS-SH) to design a double-crosslinked hydrogel for wound dressing. When crosslinked together, the resulting hydrogels showed a highly porous inner structure, and enhanced mechanical properties and moisture retention capacity. The compression modulus of the GelMA/CS-SH hydrogel (GCH) reached up to about 40 kPa and was much higher than that of pure GelMA hydrogel, and the compression modulus was increased with the amount of CS-SH. In vitro study showed no cytotoxicity of obtained hydrogels. Interestingly, a higher concentration of CS-SH slightly promoted the proliferation of cells. Moreover, the double-crosslinked hydrogel exhibited antibacterial properties because of the presence of chitosan. In vivo study based on rats showed that full-thickness skin defects healed on the 15th day. Histological results indicate that the hydrogel accelerated the repair of hair follicles and encouraged the orderly growth of collagen fibers in the wound. Furthermore, better blood vessel formation and a higher expression of VEGFR were observed in the hydrogel group when compared with the untreated control group. Based on our findings, GCH could be a promising candidate for full-thickness wound dressing.
Chondroitin sulfate (CS) derivatives are useful biomacromolecules for fabrication of biomaterials. However, chemical modifications of CS molecular structure during processing may alter its ...physicochemical and biological properties. Here, we studied these changes in molecular and biological functions following CS oxidation to different oxidation. Under ultraviolet visible (UV–Vis) spectroscopy, CS exhibited a blue shift in characteristic absorption peaks after the oxidation. The thermo-stability of the modified CS was also weaker than its original molecular form. Both FTIR and NMR results demonstrated distinct structural changes at the molecular level after oxidation. In vitro study showed that rabbit bone marrow stromal cells cultured with oxidized CS (CSA) containing cell culture medium exhibited viability comparable to normal cell culture medium for CSA concentration less than 125 mg/mL. However, CSA may also inhibit proliferation of these cells. Besides, unmodified CS could induce a chondrogenesis of stem cells, but this function was weakened after chemical modification. Interestingly, chemical modification altered physicochemical and biological properties in substitution degree-dependent manner with the highly oxidized CS exhibiting the lowest stability and chondrogenic induction. These results indicated that chemical modification of biomacromolecules, such as CS, could change both their physicochemical properties and biological functions, suggesting the need to carefully control parameters during biomaterial processing and fabrication.
•Chondroitin sulfate was chemically modified in controlled conditions to form desired chondroitin sulfate derivatives.•Chondroitin sulfate derivatives with gradient amount of aldehyde groups were obtained and characterized.•Oxidation of chondroitin sulfate could influence both its physicochemical properties and biological functions.
The treatment of full-thickness skin wounds represents a major clinical challenge, and hydrogel is regarded as a promising class of biomaterials for wound repair. Here, we present a protocol for ...preparing a photo-triggering double cross-linked, adhesive, antibacterial, and biocompatible hydrogel. We describe the steps to prepare the hydrogel and evaluate its mechanical performance, swelling kinetics, antibacterial property, biocompatibility in vitro, and therapeutic effect in vivo. This protocol is also applicable to other defect models of wound injury.
For complete details on the use and execution of this protocol, please refer to our previous work.1
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•Approaches to prepare GelNB, CSMA, and GN/CM composite hydrogels•Procedure to estimate mechanical property, swelling behavior, and antibacterial property•Steps to establish in vivo rat skin defect models•Strategy to evaluate GN/CM hydrogel therapeutic effect for skin defect
Publisher’s note: Undertaking any experimental protocol requires adherence to local institutional guidelines for laboratory safety and ethics.
The treatment of full-thickness skin wounds represents a major clinical challenge, and hydrogel is regarded as a promising class of biomaterials for wound repair. Here, we present a protocol for preparing a photo-triggering double cross-linked, adhesive, antibacterial, and biocompatible hydrogel. We describe the steps to prepare the hydrogel and evaluate its mechanical performance, swelling kinetics, antibacterial property, biocompatibility in vitro, and therapeutic effect in vivo. This protocol is also applicable to other defect models of wound injury.
Full-thickness wounds, lacking the epidermis and entire dermis and extending into subcutaneous fat, represent a common treatment challenge. Due to the loss of adnexal structures as a source of ...keratinocytes, full-thickness wounds healing can only be achieved by re-epithelialization from the wound edge and contraction. Here, we developed a hydrogel composed of chitosan methacrylate (CSMA) and o-nitrosobenzaldehyde-modified gelatin (GelNB) for promoting full-thickness wound healing. The CSMA/GelNB (CM/GN) hydrogels exhibited superior mechanical and adhesive properties than that of pure CSMA hydrogel. In vivo experiments confirmed that CM/GN could promote wound healing by generating more hair follicles and mutual blood vessels, high fibroblasts density, and thicker granulation tissue thickness. In addition, reduced secretions of tumor necrosis factor-α (TNF-α) and enhanced secretions of vascular endothelial growth factor (VEGF) could be observed in regenerated tissues after CM/GN treatment. These results suggested that CM/GN hydrogels could be promising candidates to promote wound healing.
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•The CM/GN hydrogels exhibited tissue adhesive properties•CM/GN hydrogel facilitated the proliferation of bone marrow stem cells•CM/GN hydrogel efficiently promote full-thickness wound healing•More hair follicles and mutual blood vessels were generated during wound healing
Biotechnology; Applied sciences; Bioengineering; Materials science; Biomaterials
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•Novel magnetic pullulan (MP) hydrogels were designed.•These prepared MP hydrogels were for the first time used as Fenton-like catalysts.•MP hydrogels exhibited excellent degradation ...activity, reusability and stability.•Degradation mechanism for tetracycline hydrochloride in our MP3/H2O2 system was proposed.
Magnetic nanoparticles that can be employed as Fenton-like catalysts Fenton-like catalysts are attractive materials for degrading antibiotics. In this study, we facilely prepared novel magnetic pullulan (MP) hydrogels by doping modified magnetic nanoparticles into pullulan matrices, which could enhance catalytic degradation performance and strengthen the stability of resulting hydrogels. This is the first time that MP hydrogels have been fabricated successfully and used as Fenton-like catalysts for tetracycline hydrochloride (TCH) degradation. MP hydrogels were characterized and their catalytic TCH degradation abilities were also investigated. The optimized conditions (pH value, Fe3O4 content, H2O2 content and TCH concentration) for TCH degradation were investigated. The optimized system showed excellent degradation efficiency for TCH. Further, the degradation mechanism was comprehensively studied. Finally, synthesized MP hydrogels showed impressive reusability and stability in the cycle experiment. Thus, our findings would open new possibilities to develop magnetic hydrogels in eliminating antibiotic contaminants.
This work reported the fast synthesis of magnetic polydopamine Au-Fenton catalyst (Fe3O4@PDA/Au) under UV irradiation at 365 nm. The microstructure of prepared nanocomposites was characterized by ...various techniques. The effects of several key factors (pH values, H2O2 content and TC concentration) of tetracycline (TC) degradation were evaluated. The results revealed that the TC and total organic carbon (TOC) removal rate reached up to 98.16% and 93.14% within 300 min under optimal conditions (pH 3, H2O2 80 μL, TC concentration 20 mg/L). Besides, HO radicals were generated during the Fenton-like degradation process and the plausible degradation mechanism was discussed. Moreover, Fe3O4@PDA/Au catalyst retained excellent catalytic capacity (TC removal rate 96.94% and TOC removal rate 87.69%) and exhibited fantastic stability after six cycles. Moreover, metal ions leaching was evaluated (0.023 mg/L). Altogether, the novel Fe3O4@PDA/Au Fenton-like catalyst is highly promising for wastewater management.
•Magnetic polydopamine Au NPs (Fe3O4@PDA/Au) were synthesized under UV irradiation.•Fe3O4@PDA/Au was for the first time used as Fenton-like catalyst.•Fe3O4@PDA/Au exhibited excellent degradation activity, reusability and stability.•Tetracycline degradation mechanism in our Fe3O4@PDA/Au/H2O2 system was explored.
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•We synthesized peptidomimetic FK-13 for cardiac implantable electronic devices pocket infections.•Our composite hydrogel possessed satisfactory sustained release effect on FK-13.•The ...PN-FK hydrogel exhibited broad-spectrum antibacterial capacity.•PN-FK coated CIED surfaces enhanced anti-infection and tissue regeneration capabilities in vivo.•The transcriptomic analysis revealed the cellular mechanisms and pathways influenced by PN-FK.
Elderly patients predispose to cardiovascular implantable electronic devices (CIEDs) pocket infections due to multiple comorbidities. Treating infections with the antibiotics further carry higher risks for complications, and surgical intervention can be costly when device removal and reimplantation are required, both emphasizing the importance of novel preventive strategies to minimize the incidence of pocket infections. To meet the unique needs for elderly, we constructed an CIED surface modified hydrogel which crosslinked polyethylene glycol diacrylate (PEGDA) with hyaluronic acid-nitrobenzene (HN) to form the polymeric structures that mimic the natural environment for promoting “Pocket” surrounding tissue integration and healing. Importantly, we synthesized the new peptidomimetics FK-13 derived by shortening amino acid sequence of LL-37 which is the only human cathelicidin-derived antimicrobial peptide. By incorporating FK-13 with initial PN hydrogel via Schiff base formation, the created PN-FK hydrogel exhibited broad-spectrum antimicrobial activityagainst bacteria with excellent biocompatibility and mechanical properties in a long-term release manner. In an in vitro setting, PN-FK hydrogel demonstrated the regeneration capacity by expression of Hmox1, Col5 and Col6 associated genes in fibroblasts as well as expression of Gpx1, Cdc20 and MMP9 genes in stem cells to accelerate self-renewal, collagen secretion and reconstitution of matrix components. In the following in vivo model of subcutaneous implantation, CIED-shape titanium mesh with surface modification by PN-FK hydrogel efficiently subsided over-inflammation compared to bare titanium implant, and expedited collagen deposition and angiogenesis in peri-pocket tissues within 2 weeks. These findings underscore the potential of the PN-FK hydrogel as a transformative approach to CIED postoperative management, offering a dual-action solution that combines infection resistance with tissue regeneration capabilities.
With the increasing incidence of knee osteoarthritis (KOA), the reparation of cartilage defects is gaining more attention. Given that tissue integration plays a critical role in repairing cartilage ...defects, tissue adhesive hydrogels are highly needed in clinics. We constructed a biomacromolecule-based bioadhesive matrix hydrogel and applied it to promote cartilage regeneration. The hydrogel was composed of methacrylate gelatin and N-(2-aminoethyl)-4-(4-(hydroxymethyl)-2-methoxy-5-nitroso) butyl amide modified hyaluronic acid (HANB). The methacrylate gelatin provided a stable hydrogel network as a scaffold, and the HANB served as a tissue-adhesive agent and could be favorable for the chondrogenesis of stem cells. Additionally, the chemically modified HA increased the swelling ratio and compressive modulus of the hydrogels. The results of our in vitro study revealed that the hydrogel was compatible with bone marrow stromal cells. In vivo, the hyaluronic-acid-containing hydrogels were found to promote articular cartilage regeneration in the defect site. Therefore, this biomaterial provides promising potential for cartilage repair.
•GM/HN hydrogels have stable network and tissue-adhesive properties.•Chemically modified HA increased the swelling ratio and compressive modulus of the hydrogels.•In vitro study revealed that the hydrogel was non-cytotoxic.•The gelatin/hyaluronic-acid adhesive hydrogels promoted articular cartilage regeneration in vivo.
Chitosan hydrogels with essential antibacterial properties and biocompatibility have great potential in tissue engineering and regeneration medicine. However, pure chitosan hydrogel could be limited ...by insufficient mechanical properties. In this work, we designed a multi-functional chitosan hydrogel based on the combination of chitosan methacrylate (CTSMA) and sulfhydrated chitosan (CTSSH), which is cross-linked simultaneously by free-radical polymerization reaction and Thiol-ene reaction. The CTSMA/CTSSH (CMS) hydrogels displayed superior tissue adhesive and mechanical properties when compared to pure CTSMA hydrogel. Additionally, the resulting hydrogels exhibited potent antimicrobial effects against both E. coli and S. aureus. Besides, the CMS hydrogels exhibited good biocompatibility as demonstrated by cytotoxicity and cell proliferation experiments using fibroblasts cells (L929) and adipose-derived stem cells (ADSCs). In vivo experiment, the repairing effect of hydrogels on full-thickness skin defect model in rats was studied. Histological and immunohistochemical staining results showed that CMS hydrogels promoted angiogenesis, dermal repair and epidermal regeneration. Overall, the study highlights the potential of the CMS hydrogels as a promising biomaterial in wound healing applications.
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