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univ-montp1.frResearch Topics:
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Biodegradable networks for soft tissue engineering by thiol–yne photo cross-linking of multifunctional polyesters.  Author(s): Nottelet B. (Article) Published: Rsc Advances, vol. 4 p.32017-32023 (2014) Ref HAL: hal-01091330_v1 DOI: 10.1039/c4ra03665d Abstract: Novel biodegradable networks have been prepared by combination of post-polymerization modification of poly(ε-caprolactone) and thiol–yne photo cross-linking. In a first step, a novel multifunctional poly(ε-caprolactone) bearing propargyl groups (PCL–yne, 8 mol% substitution degree) was obtained in a rapid one-pot reaction and at a multigram scale. In a second step, PCL–yne and mixtures of PCL and PCL–yne were cross-linked via photoradical thiol–yne reaction in the presence of pentaerythritol tetrakis(3-mercaptopropionate) and various photoinitiators. The thermal properties and stabilities of the obtained networks have been evaluated before assessment of their mechanical properties. Finally, biocompatibility studies are reported with evaluation of the proliferation of L929 fibroblasts on the materials. |
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Regioselective Halogenation of Poly(lactide) by Free-Radical Process
Author(s): Nottelet B. (Article) Published: Macromolecular Reaction Engineering, vol. 8 p.141-148 (2014) Ref HAL: hal-00992399_v1 DOI: 10.1002/mren.201300136 Abstract: Modification of the biodegradable and renewable poly(lactide) (PLA) to provide functional aliphatic polyesters is highly desirable to meet application requirements. In this context, the objective of this work is to evaluate the possibility of using free-radical substitution as a simple and non-degrading method to yield the desired functional PLA. Halogenation of PLA is carried out in solution and various reaction conditions are evaluated. Halogenated PLAs are characterized by 1 H NMR spectroscopy and size exclu- sion chromatography (SEC) to evaluate the substitution ratios and to check the non-degrading character of the radical modification. Furthermore, reactions on model compounds as well as MALDI-TOF analyses are per- formed to elucidate the involved mechanism. The combined results prove the free-radical halogenation of PLA in solution to be regioselective with only the v-halogenated PLA being obtained without main-chain substitution. |
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Toward potent antibiofilm degradable medical devices: A generic method for the antibacterial surface modification of polylactide Author(s): Nottelet B. (Article) Published: Acta Biomaterialia, vol. 9 p.7709-7718 (2013) Ref HAL: hal-00958350_v1 DOI: 10.1016/j.actbio.2013.04.018 Abstract: The effects of biomaterials on their environment must be carefully modulated in most biomedical applications. Among other approaches, this modulation can be obtained through the modification of the biomaterial surface. This paper proposes a simple and versatile strategy to produce non-leaching antibacterial polylactide (PLA) surfaces without any degradation of the polyester chains. The method is based on a one-pot procedure that provides a "clickable" PLA surface via anionic activation which is then functionalized with an antibacterial quaternized poly(2-(dimethylamino)ethyl methacrylate) (QPDMAEMA) by covalent immobilization on the surface. The anti-adherence and antibiofilm activities of modified PLA surfaces are assessed for different QPDMAEMA molecular weights and different quaternization agents. Antibacterial PLA surfaces are shown to be very active against Gram-negative and Gram-positive strains, with adherence reduction factors superior to 99.999% and a marked reduction in biofilm on the most potent surfaces. In addition to this substantial antibacterial activity, the proposed PLA surfaces are also cytocompatible, as demonstrated through the proliferation of L929 fibroblasts. |
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PLA-based biodegradable and tunable soft elastomers for biomedical applications Author(s): Nottelet B. (Article) Published: Biomedical Materials, vol. 6 p.1-11 (2011) Ref HAL: hal-00680814_v1 DOI: 10.1088/1748-6041/6/6/065006 Abstract: Although desirable for biomedical applications, soft degradable elastomers having balanced amphiphilic behaviour are rarely described in the literature. Indeed, mainly highly hydrophobic elastomers or very hydrophilic elastomers with hydrogel behaviours are found. In this work, we developed thermoset degradable elastomers based on the photo-cross-linking of poly(lactide)-poly(ethylene glycol)-poly(lactide) (PLA-PEG-PLA) triblock prepolymers. The originality of the proposed elastomers comes from the careful choice of the prepolymer amphiphilicity and from the possible modulation of their mechanical properties and degradation rates provided by cross-linkers of different nature. This is illustrated with the hydrophobic and rigid 2,4,6-triallyloxy-1,3,5-triazine compared to the hydrophilic and soft pentaerythritol triallyl ether. Thermal properties, mechanical properties, swelling behaviours, degradation rates and cytocompatibility have been evaluated. Results show that it is possible to generate a family of degradable elastomers covering a broad range of properties from a single biocompatible and biodegradable prepolymer. |
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Atom transfer radical coupling of polystyrene and poly(methyl acrylate) synthesized by reverse iodine transfer polymerization Author(s): Nottelet B., Lacroix-Desmazes Patrick, Boutevin Bernard (Article) Published: -Polymer, vol. 48 p.50-57 (2007) DOI: 10.1016/j.polymer.2006.11.005 Abstract: Iodo-terminated polystyrene and poly(methyl acrylate) (PMA-I) were synthesized by reverse iodine transfer polymerization. The resulting polymers were coupled by atom transfer radical coupling using Cu(I)/linear amino-ligand catalysts in the presence of reducing Cu(0). The efficiency of the coupling reaction is discussed as a function of various factors, namely, the Cu(0) particle sizes, the number of nitrogen present in the ligand structure, the type of halogen associated with Cu(I) (CuX, X = I, Br, Cl), the nature of the polymer and the nature of the chain ends. In particular, a quantitative coupling (100%) was obtained with a CuBr/HMTETA system in the presence of nanosized Cu(0) for PMA-I, thus opening for the first time a facile route to telechelic and multiblock poly(acrylate)-based structures. |