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The treatment of chronic wounds still presents great challenges due to being infected by biofilms and the damaged healing process. The current treatments do not address the needs of chronic wounds. In this study, a highly effective dressing (Dox-DFO@MN Hy) for the treatment of chronic wounds is described. This dressing combines the advantages of microneedles (MNs) and hydrogels in the treatment of chronic wounds. MNs is employed to debride the biofilms and break down the wound barrier, providing rapid access to therapeutic drugs from hydrogel backing layer. Importantly, to kill the pathogenic bacteria in the biofilms specifically, Doxycycline hydrochloride (Dox) is wrapped into the polycaprolactone (PCL) microspheres that have lipase-responsive properties and loaded into the tips of MNs. At the same time, hydrogel backing layer is used to seal the wound and accelerate wound healing. Benefiting from the combination of two advantages of MNs and hydrogel, the dressing significantly reduces the bacteria in the biofilms and effectively promotes angiogenesis and cell migration in vitro. Overall, Dox-DFO@MN Hy can effectively treat chronic wounds infected with biofilms, providing a new idea for the treatment of chronic wounds.
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Bandagens , Hidrogéis , Bactérias , Biofilmes , Movimento Celular , Antibacterianos/farmacologia , Antibacterianos/uso terapêuticoRESUMO
Diabetic chronic wounds pose significant clinical challenges due to their characteristic features of impaired extracellular matrix (ECM) function, diminished angiogenesis, chronic inflammation, and increased susceptibility to infection. To tackle these challenges and provide a comprehensive therapeutic approach for diabetic wounds, the first coaxial electrospun nanocomposite membrane is developed that incorporates multifunctional copper peroxide nanoparticles (n-CuO2 ). The membrane's nanofiber possesses a unique "core/sheath" structure consisting of n-CuO2 +PVP (Polyvinylpyrrolidone)/PCL (Polycaprolactone) composite sheath and a PCL core. When exposed to the wound's moist environment, PVP within the sheath gradually disintegrates, releasing the embedded n-CuO2 . Under a weakly acidic microenvironment (typically diabetic and infected wounds), n-CuO2 decomposes to release H2 O2 and Cu2+ ions and subsequently produce ·OH through chemodynamic reactions. This enables the anti-bacterial activity mediated by reactive oxygen species (ROS), suppressing the inflammation while enhancing angiogenesis. At the same time, the dissolution of PVP unveils unique nano-grooved surface patterns on the nanofibers, providing desirable cell-guiding function required for accelerated skin regeneration. Through meticulous material selection and design, this study pioneers the development of functional nanocomposites for multi-modal wound therapy, which holds great promise in guiding the path to healing for diabetic wounds.
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Diabetes Mellitus , Nanocompostos , Nanofibras , Humanos , Cicatrização , Pele/lesões , Nanocompostos/química , Nanofibras/química , InflamaçãoRESUMO
To address the issue of bacterial growth on fresh-cut fruits, this paper reports the synthesis of nanosized γ-cyclodextrin metal-organic frameworks (CD-MOFs) using an ultrasound-assisted method and their application as carriers of limonene for antibacterial active packaging. The effects of the processing parameters on the morphology and crystallinity of the CD-MOFs are investigated, and the results prove that the addition of methanol is the key to producing nanosized CD-MOFs. The limonene loading content of the nanosized CD-MOFs can reach approximately 170 mg g-1. The sustained-release behaviors of limonene in the CD-MOFs are evaluated. Molecular docking simulations reveal the distribution and binding sites of limonene in the CD-MOFs. CD-MOFs are deposited on the surfaces of polycaprolactone (PCL) nanofibers via an immersion method, and limonene-loaded CD-MOF@PCL nanofibers are prepared. The morphology, crystallinity, thermal stability, mechanical properties, and antibacterial activity of the nanofibers are also studied. The nanofiber film effectively inhibits bacterial growth and prolongs the shelf life of fresh-cut apples. This study provides a novel strategy for developing antibacterial active packaging materials based on CD-MOFs and PCL nanofibers.
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Frutas , Limoneno , Estruturas Metalorgânicas , Nanofibras , Poliésteres , gama-Ciclodextrinas , Limoneno/química , Limoneno/farmacologia , Nanofibras/química , Poliésteres/química , Estruturas Metalorgânicas/química , Estruturas Metalorgânicas/farmacologia , gama-Ciclodextrinas/química , Frutas/química , Terpenos/química , Terpenos/farmacologia , Antibacterianos/farmacologia , Antibacterianos/química , Simulação de Acoplamento MolecularRESUMO
Lithium metal batteries operated with high voltage cathodes are predestined for the realization of high energy storage systems, where solid polymer electrolytes offer a possibility to improve battery safety. Al2O3_PCL is introduced as promising hybrid electrolyte made from polycaprolactone (PCL) and Al2O3 nanoparticles that can be prepared in a one-pot synthesis as a random mixture of linear PCL and PCL-grafted Al2O3. Upon grafting, synergistic effects of mechanical stability and ionic conductivity are achieved. Due to the mechanical stability, manufacture of PCL-based membranes with a thickness of 50 µm is feasible, yielding an ionic conductivity of 5·10-5 S cm-1 at 60 °C. The membrane exhibits an impressive performance of Li deposition in symmetric Li||Li cells, operating for 1200 h at a constant and low overvoltage of 54 mV and a current density of 0.2 mA cm-2. NMC622 | Al2O3_PCL | Li cells are cycled at rates of up to 1 C, achieving 140 cycles at >80% state of health. The straightforward synthesis and opportunity of upscaling as well as solvent-free polymerization render the Al2O3_PCL hybrid material as rather safe, potentially sustainable and affordable alternative to conventional polymer-based electrolytes.
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INTRODUCTION: Diabetic foot infection (DFI) is one of the complications of diabetes mellitus. Clindamycin (CLY) is one of the antibiotics recommended to treat DFI, but CLY given orally and intravenously still causes many side effects. METHODS: In this study, we encapsulated CLY in a bacteria sensitive microparticle system (MP-CLY) using polycaprolactone (PCL) polymer. MP-CLY was then delivered in a separable effervescent microarray patch (MP-CLY-SEMAP), which has the ability to separate between the needle layer and separable layer due to the formation of air bubbles when interacting with interstitial fluid in the skin. RESULT: The characterization results of MP-CLY proved that CLY was encapsulated in large amounts as the amount of PCL polymer used increased, and there was no change in the chemical structure of CLY. In vitro release test results showed increased CLY release in media cultured with Staphylococcus aureus bacteria and showed controlled release. The characterization results of MPCLY-SEMAP showed that the developed formula has optimal mechanical and penetration capabilities and can separate in 56 ± 5.099 s. An ex vivo dermatokinetic test on a bacterially infected skin model showed an improvement of CLY dermatokinetic profile from MP-CLY SEMAP and a decrease in bacterial viability by 99.99%. CONCLUSION: This research offers proof of concept demonstrating the improved dermatokinetic profile of CLY encapsulated in a bacteria sensitive MP form and delivered via MP-CLY-SEMAP. The results of this research can be developed for future research by testing MP-CLY-SEMAP in vivo in appropriate animal models.
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Antibacterianos , Clindamicina , Pé Diabético , Pele , Staphylococcus aureus , Clindamicina/administração & dosagem , Pé Diabético/tratamento farmacológico , Pé Diabético/microbiologia , Antibacterianos/administração & dosagem , Antibacterianos/farmacologia , Staphylococcus aureus/efeitos dos fármacos , Animais , Pele/microbiologia , Pele/metabolismo , Poliésteres/química , Sistemas de Liberação de Medicamentos/métodos , Liberação Controlada de Fármacos , Administração Cutânea , Adesivo Transdérmico , Humanos , Infecções Estafilocócicas/tratamento farmacológico , Infecções Estafilocócicas/microbiologia , Portadores de Fármacos/químicaRESUMO
A novel method based on light-induced fabrication of a poly (3,4-ethylenedioxythiophene)-polycaprolactone (PEDOT-PCL) scaffold using phenacyl bromide (PAB) as a single-component photoinitiator is presented. HBr released from the step-growth polymerization of EDOT is utilized as an in situ catalyst for the chain-growth polymerization of ε-caprolactone. Detailed investigations disclose the formation of a self-assembled nanoporous electroconductive scaffold (1.2 mS cm-1 ). Fluorescence emission spectra of the fabricated scaffold exhibit a mixed solvatochromic behavior, indicating specific interactions between the self-assembled scaffold and solvents with varying polarities, as evidenced by transmission electron microscopy (TEM). Moreover, the same light-induced technique can also be applied for bulk photopolymerization showcasing the versatility and wide-ranging scope of the originated method. In brief, this study introduces a novel approach for light-induced polymerization reactions that is merging step-growth and chain-growth mechanisms. This innovative approach is promising to facilitate in situ polymerization of monomers possessing diverse functionalities.
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Nanoporos , Polimerização , Microscopia Eletrônica de Transmissão , SolventesRESUMO
BACKGROUND: The integration of stem cells, signaling molecules, and biomaterial scaffolds is fundamental for the successful engineering of functional bone tissue. Currently, the development of composite scaffolds has emerged as an attractive approach to meet the criteria of ideal scaffolds utilized in bone tissue engineering (BTE) for facilitating bone regeneration in bone defects. Recently, the incorporation of polycaprolactone (PCL) with hydroxyapatite (HA) has been developed as one of the suitable substitutes for BTE applications owing to their promising osteogenic properties. In this study, a three-dimensional (3D) scaffold composed of PCL integrated with HA (PCL/HA) was prepared and assessed for its ability to support osteogenesis in vitro. Furthermore, this scaffold was evaluated explicitly for its efficacy in promoting the proliferation and osteogenic differentiation of canine bone marrow-derived mesenchymal stem cells (cBM-MSCs) to fill the knowledge gap regarding the use of composite scaffolds for BTE in the veterinary orthopedics field. RESULTS: Our findings indicate that the PCL/HA scaffolds substantially supported the proliferation of cBM-MSCs. Notably, the group subjected to osteogenic induction exhibited a markedly upregulated expression of the osteogenic gene osterix (OSX) compared to the control group. Additionally, the construction of 3D scaffold constructs with differentiated cells and an extracellular matrix (ECM) was successfully imaged using scanning electron microscopy. Elemental analysis using a scanning electron microscope coupled with energy-dispersive X-ray spectroscopy confirmed that these constructs possessed the mineral content of bone-like compositions, particularly the presence of calcium and phosphorus. CONCLUSIONS: This research highlights the synergistic potential of PCL/HA scaffolds in concert with cBM-MSCs, presenting a multidisciplinary approach to scaffold fabrication that effectively regulates cell proliferation and osteogenic differentiation. Future in vivo studies focusing on the repair and regeneration of bone defects are warranted to further explore the regenerative capacity of these constructs, with the ultimate goal of assessing their potential in veterinary clinical applications.
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Regeneração Óssea , Durapatita , Células-Tronco Mesenquimais , Osteogênese , Poliésteres , Alicerces Teciduais , Animais , Cães , Poliésteres/química , Poliésteres/farmacologia , Alicerces Teciduais/química , Osteogênese/efeitos dos fármacos , Durapatita/química , Durapatita/farmacologia , Células-Tronco Mesenquimais/fisiologia , Regeneração Óssea/efeitos dos fármacos , Proliferação de Células , Diferenciação Celular/efeitos dos fármacos , Engenharia Tecidual/métodosRESUMO
The COVID-19 pandemic has raised concern regarding respiratory system diseases and oral inhalation stands out as an attractive non-invasive route of administration for pulmonary diseases such as chronic bronchitis, cystic fibrosis, COVID-19 and community-acquired pneumonia. In this context, we encapsulated azithromycin in polycaprolactone nanoparticles functionalized with phospholipids rich in dipalmitoylphosphatidylcholine and further produced a fine powder formulation by spray drying with monohydrated lactose. Nanoparticles obtained by the emulsion/solvent diffusion-evaporation technique exhibited a mean hydrodynamic diameter around 195-228 nm with a narrow monomodal size distribution (PdI < 0.2). Nanoparticle dispersions were spray-dried at different inlet temperatures, atomizing air-flow, aspirator air flow, and feed rate, using lactose as a drying aid, resulting in a maximal process yield of 63% and an encapsulation efficiency of 83%. Excipients and the dry powder formulations were characterized in terms of morphology, chemical structure, thermal analyses and particle size by SEM, FTIR, DSC/TGA and laser light diffraction. The results indicated spherical particles with 90% at 4.06 µm or below, an adequate size for pulmonary delivery. Aerosolization performance in a NGI confirmed good aerodynamic properties. Microbiological assays showed that the formulation preserves AZM antimicrobial effect against Staphylococcus aureus and Streptococcus pneumoniae strains, with halos above 18 mm. In addition, no formulation-related cytotoxicity was observed against the human cell lines BEAS-2B (lung epithelial), HUVEC (endothelial) and HFF1 (fibroblasts). Overall, the approach described here allows the production of AZM-PCL nanoparticles incorporated into inhalable microparticles, enabling more efficient pulmonary therapy of lung infections.
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Antibacterianos , Azitromicina , Nanopartículas , Tamanho da Partícula , Poliésteres , Pós , Azitromicina/administração & dosagem , Azitromicina/química , Azitromicina/farmacologia , Azitromicina/farmacocinética , Humanos , Nanopartículas/química , Antibacterianos/administração & dosagem , Antibacterianos/química , Antibacterianos/farmacologia , Administração por Inalação , Poliésteres/química , Inaladores de Pó Seco , Composição de Medicamentos , Excipientes/química , Linhagem Celular , Lactose/química , Staphylococcus aureus/efeitos dos fármacos , Secagem por Atomização , 1,2-Dipalmitoilfosfatidilcolina/química , Streptococcus pneumoniae/efeitos dos fármacosRESUMO
The osteoimmune microenvironment induced by implants plays a significant role in bone regeneration. It is essential to efficiently and timely switch the macrophage phenotype from M1 to M2 for optimal bone healing. This study examined the impact of a calcium phosphate (CaP) coating on the physiochemical properties of highly ordered polycaprolactone (PCL) scaffolds fabricated using melt electrowritten (MEW). Additionally, it investigated the influence of these scaffolds on macrophage polarization and their immunomodulation on osteogenesis. The results revealed that the CaP coated PCL scaffold exhibited a rougher surface topography and higher hydrophilicity in comparison to the PCL scaffold without coating. Besides, the surface morphology of the coating and the release of Ca2+ from the CaP coating were crucial in regulating the transition of macrophages from M1 to M2 phenotypes. They might activate the PI3K/AKT and cAMP-PKA pathways, respectively, to facilitate M2 polarization. In addition, the osteoimmune microenvironment induced by CaP coated PCL could not only enhance the osteogenic differentiation of bone marrow-derived mesenchymal stem cells (BMSCs) in vitro but also promote the bone regeneration in vivo. Taken together, the CaP coating can be employed to control the phenotypic switching of macrophages, thereby creating a beneficial immunomodulatory microenvironment that promotes bone regeneration.
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Osteogênese , Alicerces Teciduais , Alicerces Teciduais/química , Fosfatidilinositol 3-Quinases/metabolismo , Regeneração Óssea , Macrófagos/metabolismo , Fosfatos de Cálcio/químicaRESUMO
BACKGROUND: This case report demonstrates the effective clinical application of a 3D-printed, patient-specific polycaprolactone (PCL) resorbable scaffold for staged alveolar bone augmentation. OBJECTIVE: To evaluate the effectiveness of a 3D-printed PCL scaffold in facilitating alveolar bone regeneration and subsequent dental implant placement. MATERIALS AND METHODS: A 46-year-old man with a missing tooth (11) underwent staged alveolar bone augmentation using a patient-specific PCL scaffold. Volumetric bone gain and implant stability were assessed. Histological analysis was conducted to evaluate new bone formation and graft integration. RESULTS: The novel approach resulted in a volumetric bone gain of 364.69 ± 2.53 mm3, sufficient to reconstruct the original alveolar bone contour and permit dental implant placement. Histological analysis showed new bone presence and successful graft integration across all defect zones (coronal, medial, and apical), with continuous new bone formation around and between graft particles. The dental implant achieved primary stability at 35 Ncm-1, indicating the scaffold's effectiveness in promoting bone regeneration and supporting implant therapy. The post-grafting planned implant position deviated overall by 2.4° compared with the initial restoratively driven implant plan pre-bone augmentation surgery. The patient reported low average daily pain during the first 48 h and no pain from Day 3. CONCLUSIONS: This proof-of-concept underscores the potential of 3D-printed scaffolds in personalized dental reconstruction and alveolar bone regeneration. It marks a significant step forward in integrating additive manufacturing technologies into clinical practice through a scaffold-guided bone regeneration (SGBR) approach. The trial was registered with the Australian New Zealand Clinical Trials Registry (ACTRN12622000118707p).
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In this study, a novel application of synchrotron X-ray nanotomography based on high-resolution full-field transmission X-ray microscopy for characterizing the structure and morphology of micrometric hollow polymeric fibers is presented. By employing postimage analysis using an open-source software such as Tomviz and ImageJ, various key parameters in fiber morphology, including diameter, wall thickness, wall thickness distribution, pore size, porosity, and surface roughness, were assessed. Electrospun polycaprolactone fibers with micrometric diameters and submicrometric features with induced porosity via gas dissolution foaming were used to this aim. The acquired synchrotron X-ray nanotomography data were analyzed using two approaches: 3D tomographic reconstruction and 2D radiographic projection-based analysis. The results of the combination of both approaches demonstrate unique capabilities of this technique, not achievable by other available techniques, allowing for a full characterization of the internal and external morphology and structure of the fibers as well as to obtain valuable qualitative insights into the overall fiber structure.
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BACKGROUND/PURPOSE: 3D-printing technology is an important tool for the bone tissue engineering (BTE). The aim of this study was to investigate the interaction of polycaprolactone (PCL) scaffolds and modified mesh PCL coated with beta TCP (PCL/ß-TCP) scaffolds with MG-63. METHODS: This study used the fused deposition modeling (FDM) technique with the 3D printing technique to fabricate the thermoplastic polymer and composite scaffolds. Scaffold structure and coating quality were observed under a scanning electron microscope (SEM). MG-63 cells were injected and attached to the mesh-manufactured PCL scaffolds. The biocompatibility of mesh structured PCL and PCL/ß-TCP scaffolds could be examined by measuring the viability of MG-63 cells of MTT assay. Bone cell differentiation was evaluated ALP activity by mineralization assay. RESULTS: The results showed that both mesh PCL scaffolds and PCL/ß-TCP scaffolds were non-toxic to the cells. The ALP activities of cells in PCL/ß-TCP scaffolds groups were significant differences and better than PCL groups in all groups at all experimental dates. The mineralization process was time-dependent, and significantly higher mineralization of osteosarcoma cells was observed on PCL/ß-TCP scaffolds at experimental dates. CONCLUSION: We concluded that both meshes structured PCL and PCL/ß-TCP scaffolds could promote the MG-63 cell growth, and PCL/ß-TCP was better than the PCL scaffolds for the outcome of MG63 cell differentiation and mineralization.
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Regeneração Óssea , Poliésteres , Alicerces Teciduais , Humanos , Alicerces Teciduais/química , Fosfatos de Cálcio/química , Impressão TridimensionalRESUMO
OBJECTIVE: The purpose of this study was to prepare and evaluate chitosan (CS) gel containing metformin hydrochloride (MET)-loaded polycaprolactone (PCL) nanoparticles (NPs) for topical treatment of melanoma. SIGNIFICANCE: Topical administration of MET-PCL NPs-CS gel improves penetration of drug, decreases side effects, and increases efficacy of treatment. METHODS: MET-PCL NPs were prepared by double emulsion method. Particle size, charge, encapsulation efficiency (EE), release, and morphology were evaluated. MET-PCL NPs-CS gel formulation was characterized in terms of organoleptic properties, pH, gelling time, viscosity, spreadability, release, and morphology. Cytotoxicity was performed on B16F10 cells. Ex vivo permeability was done with pig skin. RESULTS: The size, charge, and EE were found to be 180 ± 10 nm, -11.4 mV, and 93%. SEM images showed that NPs were spherical and smooth. An initial burst release followed by a slower release was observed. MET-PCL NPs-CS gel was found to be transparent. The pH was 4.9 ± 0.05. The gelation time was 1.6 ± 0.2 min. The viscosity results confirm pseudoplastic behavior of gel. The spreadability by % area was 392 ± 6.4 cm. The images showed that gelling network of CS gel was composed of suspended NPs. The viscosity was between 554 and 3503 cP. MET-PCL NPs-CS gel showed prolonged release up to 72 h. On B16F10 cells, gel showed higher cytotoxicity compared to MET solution. MET-PCL NPs-CS gel had twofold higher permeability in pig skin compared with MET-CS gel. CONCLUSION: Topical administration of MET-PCL NPs-CS gel into the skin resulted in improved dermal penetration and this promising approach may be of value in effective treatment of melanoma and other skin cancers.
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Quitosana , Géis , Metformina , Nanopartículas , Tamanho da Partícula , Quitosana/química , Metformina/administração & dosagem , Metformina/química , Metformina/farmacologia , Metformina/farmacocinética , Nanopartículas/química , Animais , Géis/química , Camundongos , Suínos , Poliésteres/química , Portadores de Fármacos/química , Administração Tópica , Linhagem Celular Tumoral , Melanoma/tratamento farmacológico , Melanoma/patologia , Liberação Controlada de Fármacos , Absorção Cutânea/efeitos dos fármacos , Polímeros/química , Melanoma Experimental/tratamento farmacológico , Melanoma Experimental/patologia , Viscosidade , Pele/efeitos dos fármacos , Pele/metabolismo , Neoplasias Cutâneas/tratamento farmacológico , Neoplasias Cutâneas/patologia , Permeabilidade/efeitos dos fármacosRESUMO
Schwann cell (SC) transplantation represents a promising therapeutic approach for traumatic spinal cord injury but is frustrated by barrier formation, preventing cell migration, and axonal regeneration at the interface between grafted SCs and reactive resident astrocytes (ACs). Although regenerating axons successfully extend into SC grafts, only a few cross the SC-AC interface to re-enter lesioned neuropil. To date, research has focused on identifying and modifying the molecular mechanisms underlying such scarring cell-cell interactions, while the influence of substrate topography remains largely unexplored. Using a recently modified cell confrontation assay to model SC-AC barrier formation in vitro, highly oriented poly(ε-caprolactone) nanofibers were observed to reduce AC reactivity, induce extensive oriented intermingling between SCs and ACs, and ultimately enable substantial neurite outgrowth from the SC compartment into the AC territory. It is anticipated that these findings will have important implications for the future design of biomaterial-based scaffolds for nervous tissue repair.
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Astrócitos , Neuritos , Humanos , Axônios , Regeneração Nervosa , Cicatriz/patologia , Células de Schwann/patologia , Células de Schwann/fisiologia , Células de Schwann/transplanteRESUMO
To repair damaged mesothelium tissue, which lines internal organs and cavities, a tissue engineering approach with mesothelial cells seeded to a functional nanostructured scaffold is a promising approach. Therefore, this study explored the uses of electrospun nanofiber membrane scaffolds (NMSs) as scaffolds for mesothelial cell culture and transplantation. We fabricated a composite NMS through electrospinning by blending polycaprolactone (PCL) with gelatin. The addition of gelatin enhanced the membrane's hydrophilicity while maintaining its mechanical strength and promoted cell attachment. The in vitro study demonstrated enhanced adhesion of mesothelial cells to the scaffold with improved morphology and increased phenotypic expression of key marker proteins calretinin and E-cadherin in PCL/gelatin compared to pure PCL NMSs. In vivo studies in rats revealed that only cell-seeded PCL/gelatin NMS constructs fostered mesothelial healing. Implantation of these constructs leads to the regeneration of new mesothelium tissue. The neo-mesothelium is similar to native mesothelium from hematoxylin and eosin (H&E) and immunohistochemical staining. Taken together, the PCL/gelatin NMSs can be a promising scaffold for mesothelial cell attachment, proliferation, and differentiation, and the cell/scaffold construct can be used in therapeutic applications to reconstruct a mesothelium layer.
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Gelatina , Nanofibras , Poliésteres , Engenharia Tecidual , Alicerces Teciduais , Nanofibras/química , Gelatina/química , Alicerces Teciduais/química , Poliésteres/química , Animais , Ratos , Epitélio/efeitos dos fármacos , Engenharia Tecidual/métodos , Proliferação de Células/efeitos dos fármacos , Adesão Celular/efeitos dos fármacos , Células Epiteliais/metabolismo , Células Epiteliais/citologia , Células Cultivadas , HumanosRESUMO
The rising accumulation of poly(ethylene terephthalate) (PET) waste presents an urgent ecological challenge, necessitating an efficient and economical treatment technology. Here, we developed chemical-biological module clusters that perform chemical pretreatment, enzymatic degradation, and microbial assimilation for the large-scale treatment of PET waste. This module cluster included (i) a chemical pretreatment that involves incorporating polycaprolactone (PCL) at a weight ratio of 2% (PET:PCL = 98:2) into PET via mechanical blending, which effectively reduces the crystallinity and enhances degradation; (ii) enzymatic degradation using Thermobifida fusca cutinase variant (4Mz), that achieves complete degradation of pretreated PET at 300 g/L PET, with an enzymatic loading of 1 mg protein per gram of PET; and (iii) microbial assimilation, where Rhodococcus jostii RHA1 metabolizes the degradation products, assimilating each monomer at a rate above 90%. A comparative life cycle assessment demonstrated that the carbon emissions from our module clusters (0.25 kg CO2-eq/kg PET) are lower than those from other established approaches. This study pioneers a closed-loop system that seamlessly incorporates pretreatment, degradation, and assimilation processes, thus mitigating the environmental impacts of PET waste and propelling the development of a circular PET economy.
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Biodegradação Ambiental , Poliésteres , Polietilenotereftalatos , Polietilenotereftalatos/química , Polietilenotereftalatos/metabolismo , Poliésteres/metabolismo , Poliésteres/química , Hidrolases de Éster CarboxílicoRESUMO
In this work, diatomaceous earth (Diat) was explored as filler for polycaprolactone (PCL) to obtain composite green materials with promising viscoelastic and thermal properties. The composites were prepared by blending variable Diat amounts (5, 15 and 50 wt%) with a molten PCL matrix. The viscoelastic characteristics of PCL/Diat hybrids were studied by Dynamic Mechanical Analysis (DMA) under an oscillatory regime, while the thermal properties were determined by Differential Scanning Calorimetry (DSC) and Thermogravimetric Analysis (TGA). We detected that the presence of Diat enhances the energy storage capacity of PCL for temperatures lower than the polymer melting point. Both DMA and DSC data revealed that the PCL melting temperature is slightly affected by the Diat addition, while the TGA results showed that the thermal stability of the polymer can be significantly improved by mixing PCL with diatomaceous earth. Moreover, we observed that the dispersion of Diat into the matrix favors the crystallization process of PCL. Interestingly, the improvements of PCL properties (elasticity, thermal stability, and crystallinity) are proportional to the Diat concentration of the composites. These findings reflect the interfacial compatibility between PCL and diatomaceous earth. In conclusion, this study highlights that the preparation of PCL/Diat hybrids by melt blending is suitable for the development of composite materials for technological applications, including the remediation of air pollutants within museum environments.
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During the past two decades, tremendous progress has been made in the development of biodegradable polymeric materials for various industrial applications, including human and veterinary medicine. They are promising alternatives to commonly used non-degradable polymers to combat the global plastic waste crisis. Among biodegradable polymers used, or potentially applicable to, veterinary medicine are natural polysaccharides, such as chitin, chitosan, and cellulose as well as various polyesters, including poly(ε-caprolactone), polylactic acid, poly(lactic-co-glycolic acid), and polyhydroxyalkanoates produced by bacteria. They can be used as implants, drug carriers, or biomaterials in tissue engineering and wound management. Their use in veterinary practice depends on their biocompatibility, inertness to living tissue, mechanical resistance, and sorption characteristics. They must be designed specifically to fit their purpose, whether it be: (1) facilitating new tissue growth and allowing for controlled interactions with living cells or cell-growth factors, (2) having mechanical properties that address functionality when applied as implants, or (3) having controlled degradability to deliver drugs to their targeted location when applied as drug-delivery vehicles. This paper aims to present recent developments in the research on biodegradable polymers in veterinary medicine and highlight the challenges and future perspectives in this area.
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Quitosana , Poli-Hidroxialcanoatos , Humanos , Poliésteres , Materiais Biocompatíveis , Engenharia Tecidual , Sistemas de Liberação de MedicamentosRESUMO
A simple and efficient method for the synthesis of biodegradable, highly branched polycaprolactone (PCL) is presented. The solvent-free (bulk) reaction was carried out via ring opening polymerization (ROP), catalyzed by tin octanoate Sn(Oct)2, and it employed hyperbranched polyamide (HPPA) as a macro-initiator. The core-shell structure of the obtained products (PCL-HPPA), with the hyperbranched HPPA core and linear PCL chains as shell, was in the focus of the product characterization. 1H nuclear magnetic resonance (1H NMR) and elemental analysis confirmed the covalent incorporation of the HPPA in the products, as well as a high degree of grafting conversion of its amino functional groups. Confocal Raman Micro spectroscopy, and especially Time-of-Flight Secondary Ion Mass Spectrometry, further supported the existence of a core-shell structure in the products. Direct observation of macromolecules by means of cryogenic transmission electron microscopy, as well as gel permeation chromatography (GPC), suggested the existence of a minor 'aggregated' product fraction with multiple HPPA cores, which was attributed to transesterification reactions. Differential scanning calorimetry, as well as X-ray diffraction, demonstrated that the PCL-HPPA polymers displayed a similar degree of crystallinity to linear neat PCL, but that the branched products possessed smaller and less regular crystallites.
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Pseudomonas aeruginosa is an opportunistic bacterial pathogen that form biofilms in chronic wounds and is difficult to treat with standard treatment methods. In the present study, flavonoid quercetin-mediated CuONPs (Que-CuONPs) were successfully synthesized and incorporated in the electrospun polycaprolactone (Que-CuONPs-PCL) nanofibrous membrane to eradicate the burn wound infection causing P. aeruginosa biofilm. The fabricated scaffold Que-CuONPs-PCL was characterized using HR-SEM, EDX, XRD, and FTIR. The synthesized Que-CuONPs appeared as spherical in shape with the average size of 36 nm. The crystallite size of the synthesized CuONPs was calculated as 23 nm. Antibacterial activity results shows that the ZOI and MIC of Que-CuONPs against P. aeruginosa was found to be 20 mm and 5 µg/mL, respectively. Antibiofilm assay results indicate the pre-formed P. aeruginosa biofilm was completely eradicated by Que-CuONPs at 8-MIC. The Que-CuONPs-PCL nanofibrous scaffolds exhibits less cytotoxic effects on mouse fibroblast (L929) cells. Finally, this study highlights the fabricated Que-CuONPs-PCL nanofibrous scaffolds exhibits an excellent antibiofilm effect against P. aeruginosa biofilm with a great biocompatibility.