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Synthesis And Characterization of Silk Fibroin-Based Hydrogels for Biomedical Applications

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Resumo:Hydrogels derived from natural polymers have garnered significant attention in biomedical fields such as Tissue Engineering (TE) and drug delivery, due to their excellent biocompatibility and biodegradability. However, these materials have some disadvantages that limit their applicability in these areas, such as low mechanical strength. These shortcomings can be overcome by introducing a secondary polymeric network to create a hydrogel with improved mechanical properties. This work aimed to construct hydrogels composed of two networks using only natural polymers, with improved mechanical properties compared to natural single-network hydrogels. Silk fibroin (SF) was selected as the foundation of the primary network due to its inherent superior mechanical properties and high biocompatibility. To form a more robust network, the SF was functionalized through methacrylation, obtaining methacrylated silk fibroin (SFMA), a photo-cross-linkable polymer. The polymers selected for comprising the secondary network were gelatin methacrylate (GelMa), and alginate (SA). To obtain GelMagelatin was also functionalized by methacrylation. The combination of these polymers results in covalently cross-linked SFMA/GelMa hydrogels and SFMA/SA hydrogels withcovalent/ionic cross-linking. The formulations constituting these hydrogels were optimized throughout the study by evaluating the results obtained by rheological testing, as well as critical observation of the fabrication of these materials. The SFMA/GelMa hydrogels, characterized by networks cross-linked by covalent bonds, were more resistant to deformation, having reached a maximum elastic modulus (G') value of 4200 Pa. The SFMA/SA hydrogels reached a maximum G' of 2344 Pa in the linear viscoelasticity region. These results were corroborated by uniaxial compression tests, in which the SFMA/GelMa formulations tested exhibited greaterrigidity. The SFMA/GelMa 20/15% (w/v) and SFMA/SA 20/1 % (w/v) formulations obtained a compressive elastic modulus at 5% deformation of 127,9 kPa and 65,68 kPa, respectively.The developed hydrogels show promising results, as evidenced by improved mechanical properties. These improvements, particularly in the SFMA/GelMa hydrogels, make them suitable candidates for biomedical applications that require enhanced structural robustness.
Autores principais:Marcelino, João Pedro Pedrosa
Assunto:Natural Hydrogels Polymers Silk fibroin methacrylate Tissue Engineering Rheology Hidrogéis naturais Polímeros Fibroína da seda metacrilada Engenharia de tecidos Reologia
Ano:2024
País:Portugal
Tipo de documento:dissertação de mestrado
Tipo de acesso:acesso embargado
Instituição associada:Universidade de Coimbra
Idioma:inglês
Origem:Estudo Geral - Universidade de Coimbra
Descrição
Resumo:Hydrogels derived from natural polymers have garnered significant attention in biomedical fields such as Tissue Engineering (TE) and drug delivery, due to their excellent biocompatibility and biodegradability. However, these materials have some disadvantages that limit their applicability in these areas, such as low mechanical strength. These shortcomings can be overcome by introducing a secondary polymeric network to create a hydrogel with improved mechanical properties. This work aimed to construct hydrogels composed of two networks using only natural polymers, with improved mechanical properties compared to natural single-network hydrogels. Silk fibroin (SF) was selected as the foundation of the primary network due to its inherent superior mechanical properties and high biocompatibility. To form a more robust network, the SF was functionalized through methacrylation, obtaining methacrylated silk fibroin (SFMA), a photo-cross-linkable polymer. The polymers selected for comprising the secondary network were gelatin methacrylate (GelMa), and alginate (SA). To obtain GelMagelatin was also functionalized by methacrylation. The combination of these polymers results in covalently cross-linked SFMA/GelMa hydrogels and SFMA/SA hydrogels withcovalent/ionic cross-linking. The formulations constituting these hydrogels were optimized throughout the study by evaluating the results obtained by rheological testing, as well as critical observation of the fabrication of these materials. The SFMA/GelMa hydrogels, characterized by networks cross-linked by covalent bonds, were more resistant to deformation, having reached a maximum elastic modulus (G') value of 4200 Pa. The SFMA/SA hydrogels reached a maximum G' of 2344 Pa in the linear viscoelasticity region. These results were corroborated by uniaxial compression tests, in which the SFMA/GelMa formulations tested exhibited greaterrigidity. The SFMA/GelMa 20/15% (w/v) and SFMA/SA 20/1 % (w/v) formulations obtained a compressive elastic modulus at 5% deformation of 127,9 kPa and 65,68 kPa, respectively.The developed hydrogels show promising results, as evidenced by improved mechanical properties. These improvements, particularly in the SFMA/GelMa hydrogels, make them suitable candidates for biomedical applications that require enhanced structural robustness.

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