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Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties

In situ-forming gels with self-assembling and self-healing properties are materials of high interest for various biomedical applications, especially for drug delivery systems and tissue regeneration. The main goal of this research was the development of an innovative gel carrier based on dynamic int...

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Autores principales: Gradinaru, Luiza Madalina, Bercea, Maria, Lupu, Alexandra, Gradinaru, Vasile Robert
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10096672/
https://www.ncbi.nlm.nih.gov/pubmed/37050311
http://dx.doi.org/10.3390/polym15071697
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author Gradinaru, Luiza Madalina
Bercea, Maria
Lupu, Alexandra
Gradinaru, Vasile Robert
author_facet Gradinaru, Luiza Madalina
Bercea, Maria
Lupu, Alexandra
Gradinaru, Vasile Robert
author_sort Gradinaru, Luiza Madalina
collection PubMed
description In situ-forming gels with self-assembling and self-healing properties are materials of high interest for various biomedical applications, especially for drug delivery systems and tissue regeneration. The main goal of this research was the development of an innovative gel carrier based on dynamic inter- and intramolecular interactions between amphiphilic polyurethane and peptide structures. The polyurethane architecture was adapted to achieve the desired amphiphilicity for self-assembly into an aqueous solution and to facilitate an array of connections with peptides through physical interactions, such as hydrophobic interactions, dipole-dipole, electrostatic, π–π stacking, or hydrogen bonds. The mechanism of the gelation process and the macromolecular conformation in water were evaluated with DLS, ATR-FTIR, and rheological measurements at room and body temperatures. The DLS measurements revealed a bimodal distribution of small (~30–40 nm) and large (~300–400 nm) hydrodynamic diameters of micelles/aggregates at 25 °C for all samples. The increase in the peptide content led to a monomodal distribution of the peaks at 37 °C (~25 nm for the sample with the highest content of peptide). The sol–gel transition occurs very quickly for all samples (within 20–30 s), but the equilibrium state of the gel structure is reached after 1 h in absence of peptide and required more time as the content of peptide increases. Moreover, this system presented self-healing properties, as was revealed by rheological measurements. In the presence of peptide, the structure recovery after each cycle of deformation is a time-dependent process, the recovery is complete after about 300 s. Thus, the addition of the peptide enhanced the polymer chain entanglement through intermolecular interactions, leading to the preparation of a well-defined gel carrier. Undoubtedly, this type of polyurethane/peptide-based carrier, displaying a sol–gel transition at a biologically relevant temperature and enhanced viscoelastic properties, is of great interest in the development of medical devices for minimally invasive procedures or precision medicine.
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spelling pubmed-100966722023-04-13 Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties Gradinaru, Luiza Madalina Bercea, Maria Lupu, Alexandra Gradinaru, Vasile Robert Polymers (Basel) Article In situ-forming gels with self-assembling and self-healing properties are materials of high interest for various biomedical applications, especially for drug delivery systems and tissue regeneration. The main goal of this research was the development of an innovative gel carrier based on dynamic inter- and intramolecular interactions between amphiphilic polyurethane and peptide structures. The polyurethane architecture was adapted to achieve the desired amphiphilicity for self-assembly into an aqueous solution and to facilitate an array of connections with peptides through physical interactions, such as hydrophobic interactions, dipole-dipole, electrostatic, π–π stacking, or hydrogen bonds. The mechanism of the gelation process and the macromolecular conformation in water were evaluated with DLS, ATR-FTIR, and rheological measurements at room and body temperatures. The DLS measurements revealed a bimodal distribution of small (~30–40 nm) and large (~300–400 nm) hydrodynamic diameters of micelles/aggregates at 25 °C for all samples. The increase in the peptide content led to a monomodal distribution of the peaks at 37 °C (~25 nm for the sample with the highest content of peptide). The sol–gel transition occurs very quickly for all samples (within 20–30 s), but the equilibrium state of the gel structure is reached after 1 h in absence of peptide and required more time as the content of peptide increases. Moreover, this system presented self-healing properties, as was revealed by rheological measurements. In the presence of peptide, the structure recovery after each cycle of deformation is a time-dependent process, the recovery is complete after about 300 s. Thus, the addition of the peptide enhanced the polymer chain entanglement through intermolecular interactions, leading to the preparation of a well-defined gel carrier. Undoubtedly, this type of polyurethane/peptide-based carrier, displaying a sol–gel transition at a biologically relevant temperature and enhanced viscoelastic properties, is of great interest in the development of medical devices for minimally invasive procedures or precision medicine. MDPI 2023-03-29 /pmc/articles/PMC10096672/ /pubmed/37050311 http://dx.doi.org/10.3390/polym15071697 Text en © 2023 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Gradinaru, Luiza Madalina
Bercea, Maria
Lupu, Alexandra
Gradinaru, Vasile Robert
Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title_full Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title_fullStr Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title_full_unstemmed Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title_short Development of Polyurethane/Peptide-Based Carriers with Self-Healing Properties
title_sort development of polyurethane/peptide-based carriers with self-healing properties
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10096672/
https://www.ncbi.nlm.nih.gov/pubmed/37050311
http://dx.doi.org/10.3390/polym15071697
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