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Open AccessArticle Bioactive and Bioadhesive Catechol Conjugated Polymers for Tissue Regeneration
Polymers 2018, 10(7), 768; https://doi.org/10.3390/polym10070768
Received: 7 June 2018 / Revised: 3 July 2018 / Accepted: 11 July 2018 / Published: 13 July 2018
PDF Full-text (2646 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
The effective treatment of chronic wounds constitutes one of the most common worldwide healthcare problem due to the presence of high levels of proteases, free radicals and exudates in the wound, which constantly activate the inflammatory system, avoiding tissue regeneration. In this study,
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  • 817| 622| 998| 971| 7| 20| 390| 728| 324| 94| [...] Read more.
    The effective treatment of chronic wounds constitutes one of the most common worldwide healthcare problem due to the presence of high levels of proteases, free radicals and exudates in the wound, which constantly activate the inflammatory system, avoiding tissue regeneration. In this study, we describe a multifunctional bioactive and resorbable membrane with in-built antioxidant agent catechol for the continuous quenching of free radicals as well as to control inflammatory response, helping to promote the wound-healing process. This natural polyphenol (catechol) is the key molecule responsible for the mechanism of adhesion of mussels providing also the functionalized polymer with bioadhesion in the moist environment of the human body. To reach that goal, synthesized statistical copolymers of N-vinylcaprolactam (V) and 2-hydroxyethyl methacrylate (H) have been conjugated with catechol bearing hydrocaffeic acid (HCA) molecules with high yields. The system has demonstrated good biocompatibility, a sustained antioxidant response, an anti-inflammatory effect, an ultraviolet (UV) screen, and bioadhesion to porcine skin, all of these been key features in the wound-healing process. Therefore, these novel mussel-inspired materials have an enormous potential for application and can act very positively, favoring and promoting the healing effect in chronic wounds. Full article
    (This article belongs to the Special Issue Polymers for Therapy and Diagnostics)
    Figures

    Graphical abstract

    Graphical abstract
    Full article ">Figure 1
    <p>Tridimensional diagram showing the variation of instantaneous H copolymer molar fraction as a function of conversion and H feed molar fraction. Red lines represent reaction course for H feed compositions used in this work (0.2 and 0.4 mol %).</p>
    Full article ">Figure 2
    <p>Scheme of the synthesis of the acid chloride derivative of hydrocaffeic acid (HCA), VH copolymers and the catechol conjugated polymers VHC.</p>
    Full article ">Figure 3
    <p>Atomic force microscopy (AFM) (<bold>left</bold>) and scanning electron microscopy (SEM) (<bold>right</bold>) images of (<bold>a</bold>) VHC2 terpolymer and (<bold>b</bold>) VHC22 terpolymer.</p>
    Full article ">Figure 4
    <p>In vitro degradation kinetics of VHC films in Dulbecco’s modified Eagle’s medium (DMEM) (pH = 7.4) at 37 °C. Data are presented as mean ± standard deviation (<italic>n</italic> = 3).</p>
    Full article ">Figure 5
    <p>(<bold>a</bold>) Application of the polymer solution on the porcine tissue and skin samples attached each other. (<bold>b</bold>) Comparative studies in adhesion forces between the catechol conjugated polymers VHC2 and VHC22. Each line represents the stress-displacement representative curve of the two compositions after four replicates. (<bold>c</bold>) Detachment stress of the catechol containing polymers VHC2 and VHC22. Significant differences are denoted in the graph comparing the two groups at the significance level of *** <italic>p</italic> &lt; 0.001.</p>
    Full article ">Figure 6
    <p>(<bold>a</bold>) Porcine skin samples irradiated with the terpolymer film (left) and after removing the terpolymer film (right). (<bold>b</bold>) Water contact angle images of the irradiated skin under de terpolymer film (left) and of the nude irradiated skin (right). (<bold>c</bold>) Water contact angle results of the skin control (non-irradiated and irradiated) and the skin under the VHC films. Significant differences are denoted in the graph comparing the values of the irradiated samples under the VHC films and the irradiated control skin (*** <italic>p</italic> &lt; 0.001).</p>
    Full article ">Figure 7
    <p>Cell viability of human bone marrow mesenchymal stem cells (hBMSCs) treated with medium extracts of VHC films taken at different times. The diagrams include the mean and the standard deviation (<italic>n</italic> = 8).</p>
    Full article ">Figure 8
    <p>Intracellular reactive oxygen species (ROS) activity in hBMSCs measured from fluorescence emission at different times after treatment with VHC films extracts collected at 24 h. The diagrams include the mean, the standard deviation (<italic>n</italic> = 4) and the analysis of variance (ANOVA) between the different groups and the positive control at each time (* <italic>p</italic> &lt; 0.05, ** <italic>p</italic> &lt; 0.01, *** <italic>p</italic> &lt; 0.001).</p>
    Full article ">Figure 9
    <p>Inhibitory effects of VHC terpolymers on nitric oxide production in lipopolysaccharide (LPS) stimulated RAW 264.7 cells (bars) and cellular viability (lines and symbols).</p>
    Full article ">
    Open AccessFeature PaperArticle Bioactive Sr(II)/Chitosan/Poly(ε-caprolactone) Scaffolds for Craniofacial Tissue Regeneration. In Vitro and In Vivo Behavior
    Polymers 2018, 10(3), 279; https://doi.org/10.3390/polym10030279
    Received: 31 January 2018 / Revised: 23 February 2018 / Accepted: 2 March 2018 / Published: 7 March 2018
    PDF Full-text (22538 KB) | HTML Full-text | XML Full-text | Supplementary Files
    Abstract
    In craniofacial tissue regeneration, the current gold standard treatment is autologous bone grafting, however, it presents some disadvantages. Although new alternatives have emerged there is still an urgent demand of biodegradable scaffolds to act as extracellular matrix in the regeneration process. A potentially
    [...] Read more.
    In craniofacial tissue regeneration, the current gold standard treatment is autologous bone grafting, however, it presents some disadvantages. Although new alternatives have emerged there is still an urgent demand of biodegradable scaffolds to act as extracellular matrix in the regeneration process. A potentially useful element in bone regeneration is strontium. It is known to promote stimulation of osteoblasts while inhibiting osteoclasts resorption, leading to neoformed bone. The present paper reports the preparation and characterization of strontium (Sr) containing hybrid scaffolds formed by a matrix of ionically cross-linked chitosan and microparticles of poly(ε-caprolactone) (PCL). These scaffolds of relatively facile fabrication were seeded with osteoblast-like cells (MG-63) and human bone marrow mesenchymal stem cells (hBMSCs) for application in craniofacial tissue regeneration. Membrane scaffolds were prepared using chitosan:PCL ratios of 1:2 and 1:1 and 5 wt % Sr salts. Characterization was performed addressing physico-chemical properties, swelling behavior, in vitro biological performance and in vivo biocompatibility. Overall, the composition, microstructure and swelling degree (≈245%) of scaffolds combine with the adequate dimensional stability, lack of toxicity, osteogenic activity in MG-63 cells and hBMSCs, along with the in vivo biocompatibility in rats allow considering this system as a promising biomaterial for the treatment of craniofacial tissue regeneration. Full article
    (This article belongs to the Special Issue Advances in Chitin/Chitosan Characterization and Applications)
    Figures

    Graphical abstract

    Graphical abstract
    Full article ">Figure 1
    <p>EDS chemical element percent mass of Sr/Ch/2PCL and Sr/Ch/PCL dried samples. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 2
    <p>SEM images of dried blank and Sr(II) samples. (<bold>a</bold>) 250×; (<bold>b</bold>) 500×. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 3
    <p>TGA (Termogravimetric analysis) (<bold>a</bold>) and DTG (Derivative Thermogravimetric analysis) curves (<bold>b</bold>) of blank and Sr(II) membranes under nitrogen atmosphere. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 4
    <p>Variation of water uptake of membranes after immersion in PBS buffer at 37 °C. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 5
    <p>SEM images of MG-63 cells colonization on Sr(II) and blank membrane scaffolds at different post-seeding times. (<bold>a</bold>) Ch/2PCL; (<bold>b</bold>) Ch/PCL; (<bold>c</bold>) Sr/Ch/2PCL and (<bold>d</bold>) Sr/Ch/ PCL. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 6
    <p>Alamar Blue results for blank and Sr(II) membranes in MG-63 cells over a period of 21 days. Results are given as mean ± sd (<italic>n</italic> = 5). Asterisks (*) indicate a significant difference comparing the corresponding Sr(II) and blank groups at the same time (* <italic>p</italic> &lt; 0.05). Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 7
    <p>ALP/DNA activity in MG-63 cells cultured directly on test materials over a period of 14 days. Results are the mean ± sd (<italic>n</italic> = 5). Asterisks (*) indicate a significant difference comparing the two groups at the same time (* <italic>p</italic> &lt; 0.05). Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 8
    <p>SEM images of hBMSCs colonization on blank and Sr(II) scaffolds at different times post-seeding. (<bold>a</bold>) Ch/PCL and (<bold>b</bold>) Sr/Ch/PCL. Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 9
    <p>(<bold>a</bold>) Cell proliferation results obtained in AB assay of hBMSCs culture directly on test materials over a period of 21 days; (<bold>b</bold>) DNA (μg/mL) in cell lysate over a period of 14 days; (<bold>c</bold>) ALP/DNA activity over a period of 14 days. Results are the mean ± sd (<italic>n</italic> = 4). Asterisks (*) indicate a significant difference comparing blank and Sr(II) samples at the same time (* <italic>p</italic> &lt; 0.05). Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 10
    <p>Micrographs of rat subcutaneous tissue responses to Control, Ch/PCL and Sr/Ch/PLC membranes after different implantation times (7, 14 and 28 days). M: membrane, N: necrotic tissue, F: fibrous tissue, C: calcification (H-E, 4×, scale bar 1 mm). Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">Figure 11
    <p>Micrographs of rat subcutaneous tissue responses to Control, Ch/PCL and Sr/Ch/PLC membranes after different implantation times (7, 14 and 28 days). M: membrane; N: necrotic tissue; F: fibrous tissue; V: blood vessels; →: macrophages; <bold>*</bold>: multinucleated cells; +: mast cells; <bold>?</bold>: lymphocytes; ?: eosinophils; <bold>○</bold>: plasmatic cells; ?: monocytes; <bold>?</bold>: leucocytes; PMN: polymorph nuclear cells. (H-E, 20×, scale bar 100 μm). Ch: chitosan; PCL: poly(ε-caprolactone).</p>
    Full article ">

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