References of "Detrembleur, Christophe"
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See detailSynthesis of star and H-shape polymers via a combination of cobalt-mediated radical polymerization and nitrone mediated radical coupling reactions
Detrembleur, Christophe ULg; Debuigne, Antoine ULg; Altintas, Ozcan et al

in Polymer Chemistry (2012), 3(1), 135-147

Via consecutive cobalt-mediated radical polymerization (CMRP), nitrone-mediated radical coupling (NMRC) and copper catalyzed azide-alkyne cycloaddition (CuAAC), polymers with mikto-arm star and H-shape ... [more ▼]

Via consecutive cobalt-mediated radical polymerization (CMRP), nitrone-mediated radical coupling (NMRC) and copper catalyzed azide-alkyne cycloaddition (CuAAC), polymers with mikto-arm star and H-shape architecture were synthesized. Poly(vinyl acetate)40-block-poly(acrylonitrile)78-Co(acac)2 polymers were synthesized via CMRC and subsequently coupled using an alkyne functional nitrone. The coupling efficiency of the NMRC process was assessed employing N-tert-butyl a-phenyl nitrone (PBN), which is structurally very similar to the later employed coupling agent. Generally, coupling efficiencies of close to 90% or higher were observed in all cases. Since the coupling reaction yields triblock copolymers bearing an alkoxyamine functionality (and thus also an alkyne group) in the middle of the chain, well defined PEG conjugates could be obtained via CuAAC. Miktoarm star polymers of the structure (PVAc-b-PAN)2-PEG were generated as well as H-shaped material of the structure (PVAc-b-PAN)2-PEG-(PVAc-b-PAN)2 via conjugation with bifunctional PEG. In all cases, very narrow molecular weight material was obtained. Molecular weight analysis of the intermediate and the final products reveals that the hydrodynamic volume of the miktoarm star and the H-shaped materials is not substantially increased during the final conjugation reaction despite the fact that the absolute molecular weight increases by more than a factor of two in the latter case. Success of the conjugation reactions was confirmed via composition analysis via NMR. [less ▲]

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See detailKey role of intramolecular metal chelation and hydrogen bonding in the cobalt-mediated radical polymerization of N-vinyl amides
Debuigne, Antoine ULg; Morin, Aurélie; Kermagoret, Anthony ULg et al

in Chemistry : A European Journal (2012), 18

This work reveals the preponderance of an intramolecular metal chelation phenomenon in a controlled radical polymerization system involving the reversible trapping of the radical chains by a cobalt ... [more ▼]

This work reveals the preponderance of an intramolecular metal chelation phenomenon in a controlled radical polymerization system involving the reversible trapping of the radical chains by a cobalt complex, i.e. the bis(acetylacetonato)cobalt(II). The cobalt-mediated radical polymerization (CMRP) of a series of N-vinyl amides was considered in order to evidence the effect of the cobalt chelation by the amide moiety of the last monomer unit of the chain. The latter reinforces the cobalt-polymer bond in the order N-vinylpyrrolidone < N-vinyl caprolactam < N-methyl-N-vinyl acetamide, and is responsible for the optimal control of the polymerizations observed for the last two monomers. Such a double linkage between the controlling agent and the polymer, via a covalent bond and a dative one, is unique in the field of controlled radical polymerization and represents a powerful opportunity to fine tune the equilibrium between latent and free radicals. The possible hydrogen bond formation is also taken into account in the case of N-vinyl acetamide and N-vinyl formamide. These results are essential for understanding factors influencing a Co-C bond strength in general, and the CMRP mechanism in particular, but also for developing a powerful platform for the synthesis of new precision poly(N-vinyl amide)s, an important class of polymers which sustains numerous applications today. [less ▲]

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See detailCobalt-mediated radical polymerization
Debuigne, Antoine ULg; Jérôme, Robert ULg; Jérôme, Christine ULg et al

in Schlüter, Dieter A.; Hawker, Craig; Sakamoto, Junji (Eds.) Synthesis of polymers: new structures and methods (2012)

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See detailNew glucose-responsive polyelectrolyte microcapsules
Alaimo, David ULg; Detrembleur, Christophe ULg; Auzély-Velty, Rachel et al

Poster (2011, December 06)

Diabetes is a disorder of glucose regulation, characterized by an accumulation of glucose in the blood. The breakdown of glucose regulation can be attributed to the pancreas’s inability to secrete insulin ... [more ▼]

Diabetes is a disorder of glucose regulation, characterized by an accumulation of glucose in the blood. The breakdown of glucose regulation can be attributed to the pancreas’s inability to secrete insulin or to the body’s inability to properly use it. The usual treatment for type 1 diabetes consists in multiple subcutaneous insulin injections, daily administered using needles, insulin pen or insulin pump. However, this method doesn’t maintain normoglycemia and can lead to complications such as limb amputation, blindness, and kidney failure. To avoid such abnormal episodes, scientists imagined smart systems which are able to regulate the glucose level by themselves. During the past decades, a large variety of micro- and nanocarriers have been developed in order to improve efficiency, availability and toxicity profiles of drugs. In this field, stimuli-responsive polymer multilayers have attracted great scientific interest because of their potential applications as controlled delivery or release systems, for chemicals and drugs. A category of stimuli-responsive materials is able to sense glucose and respond to it by a modification of their porosity, leading to a release of insulin. The objective of this work was to investigate the formation of glucose responsive hollow microcapsules (5 microns) made of polyelectrolyte copolymers. These copolymers are composed of carbohydrate-sensitive functions, such as boronic acid and diols (PVOH), known for forming reversible covalent ether bond. In presence of carbohydrates such as glucose, the ether bonds will be reversibly broken and, consequently, the porosity of the glucose particles will change. Therefore, polyelectrolyte copolymers were synthesized by control radical polymerization, i.e. reversible addition-fragmentation chain transfer (RAFT, polyboronic acid) and cobalt-mediated radical polymerization (CMRP, PVOH). Using these polyelectrolytes as polyanions and poly(allylamine) (PAH) as a polycation, we undertook the formation of layer-by-layer capsules starting with a template of CaCO3microparticles which can be dissolved with EDTA leading to the formation of hollow microcapsules. Bovin serum albumin isothiocyanate (BSA-FITC) was used to fill the CaCO3microparticles and to determine the porosity of the resulting capsules in function of the glucose concentration. The sugar-dependent porosity is investigated by following the release of encapsulated BSA-FITC by spectro-fluoroscopy. [less ▲]

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See detailCharged poly(D,L-lactide) nanofibers: towards customized surface properties
Croisier, Florence ULg; Aqil, Abdelhafid ULg; Malherbe, Cédric ULg et al

in Macromolecular Symposia (2011), 309/310(1), 20-27

Surface-charged nanofibers were prepared by electrospinning technique (ESP). For this purpose, a copolymer bearing carboxylic acid functions was added to a poly(D,L-lactide) solution just before ESP ... [more ▼]

Surface-charged nanofibers were prepared by electrospinning technique (ESP). For this purpose, a copolymer bearing carboxylic acid functions was added to a poly(D,L-lactide) solution just before ESP process. In a basic medium, negative charges were therefore revealed on fiber surface. By deposition of positively charged particles or polyelectrolytes, surface properties of the fibers could be tailor-made for a specific application. This versatile method can, for example, be applied to the preparation of new biomedical scaffolds. [less ▲]

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See detailCaractérisation microstructurale de mousses polymères nanocomposites par microtomographie à rayons X
Plougonven, Erwan ULg; Tran, Minh Phuong ULg; Marchot, Pierre ULg et al

Poster (2011, November 29)

Les circuits électriques, fonctionnant à des fréquences de plus en plus élevées, sont responsables de l’augmentation de la pollution électromagnétique, et justifient le développement de blindages ... [more ▼]

Les circuits électriques, fonctionnant à des fréquences de plus en plus élevées, sont responsables de l’augmentation de la pollution électromagnétique, et justifient le développement de blindages efficaces. De nombreuses applications sont concernées, que ce soit dans les systèmes électroniques commerciaux, industriels, ou militaires, ou les systèmes antennaires. Récemment, des blindages sous forme de composites polymère/charges carbonées ont été largement développés pour leur nombreux avantages : plus légers, moins chers, plus absorbants, et plus facilement moulables. Une charge carbonée prometteuse est le nanotube de carbone car de par son facteur de forme, une concentration moindre est nécessaire pour une conductivité équivalente [1]. Afin d’améliorer l’absorption de l’énergie électromagnétique de ces composites (par rapport à leur réflectivité), ils sont moussés pour réduire leur constante diélectrique. Cette étape de moussage doit être rigoureusement contrôlée pour atteindre le niveau d’absorption ciblé. Deux techniques de moussage sont envisagées dans cette étude, à savoir le moussage en CO2 supercritique (par imprégnation de CO2 en condition supercritique, avant une dépressurisation rapide) et le freeze-drying (dissolution dans un solvant, suivi d’une lyophilisation de celui-ci). Ces deux méthodes génèrent des structures de porosité bien distinctes, avec une anisotropie apparente marquée dans le second cas. L’objectif est de caractériser ces structures par tailles moyennes de pores et mesures d’anisotropie, et leur lien avec l’efficacité de blindage. Dans cette optique, la caractérisation est effectuée par microtomographie à rayons X, une technique d’imagerie 3D non-destructive. Des acquisitions sont faites sur chaque échantillon, et la microstructure est analysée par traitement d’images. Vu la très faible atténuation des rayons X dans ce type de matériaux, et la limite de résolution de cette technique par rapport à la taille des pores et à l’épaisseur des parois, la séparation précise des pores par rapport à la matrice polymère s’avère difficile. Une segmentation classique n’étant pas applicable en préalable à des mesures quantitatives, la fonction d’autocorrélation est utilisée. Cette technique, habituellement utilisée en traitement du signal, est une méthode performante de mesure globale de l’anisotropie d’un matériau [2]. Elle permet également d’extraire une longueur caractéristique qui peut être liée à la taille des cellules. Les résultats mettent en évidence l’impact de la technique et des conditions de moussage sur la microstructure des mousses composites. [less ▲]

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See detailChitosan-based nanofibers with multilayered structure for wound healing application
Croisier, Florence ULg; Detrembleur, Christophe ULg; Jérôme, Christine ULg

Poster (2011, November 21)

Chitosan is a natural polymer that intrinsically presents haemostatic, mucoadhesive, antimicrobial and immunostimulant properties. This polysaccharide has shown a great potential for biomedical ... [more ▼]

Chitosan is a natural polymer that intrinsically presents haemostatic, mucoadhesive, antimicrobial and immunostimulant properties. This polysaccharide has shown a great potential for biomedical applications, on account of its remarkable compatibility with physiological medium and its biodegradability. In this respect, nanometric fibers are highly interesting as their assembly mimics the skin extracellular matrix structure. Such nanofibrous materials can be prepared by electrospinning (ESP) and can be used as scaffolds, a.o. to form a temporary, artificial extracellular matrix. In the present study, electrospinning technique was combined with layer-by-layer deposition method (LBL) – a well-known method for surface coating, based on electrostatic interactions – in order to prepare multilayered chitosan-based nanofibers for wound healing application. [less ▲]

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See detailStabilization of gold nanoparticles by thermo-responsive poly (vinyl alcohol)-b-poly (N-vinylcaprolactam) copolymers
Liu, Ji ULg; Hurtgen, Marie ULg; Detrembleur, Christophe ULg et al

Poster (2011, November 21)

Stimuli-responsive nano-materials have been playing increasingly important roles in the biomedical field due to their ability to alter the physico-chemical properties in response to external stimuli, such ... [more ▼]

Stimuli-responsive nano-materials have been playing increasingly important roles in the biomedical field due to their ability to alter the physico-chemical properties in response to external stimuli, such as temperature, pH, ionic strength, magnetic field, etc. Nanohybrids bearing an inorganic core and thermo-responsive polymer shell are particularly applicable in target delivery and controlled drug release. Poly (N-vinylcaprolactam) (PNVCL) and its copolymers, exhibiting lower critical solution temperature (LCST) where the transition between hydrophilic and hydrophobic state happens, is one of the optimal choices for this core/shell structure. Here we present the in-situ fabrication of thermo-responsive gold nanohybrids coated with a novel poly(vinyl alcohol)-b-poly(N-vinylcaprolactam) (PVOH-b-PNVCL) block copolymer prepared by the cobalt-mediated radical polymerization (CMRP). The interaction between both PVOH and PNVCL segments and gold nanoparticles was confirmed by FT-IR spectra. A sharp thermo-induced phase transition with a good reversibility upon change in temperature was detected by DLS and UV/vis spectrometer. Furthermore, the presence of hydrophilic PVOH moieties endows the gold nanohybrids with improved colloidal stability above LCST without any flocculation detected, compared with the gold nanoparticles stabilized with PNVCL homopolymer. This kind of gold nanohybrids can be envisaged as a new drug delivery vehicle. [less ▲]

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See detailNew functional poly(N-vinylpyrrolidone) based (co)polymers via photoinitiated cobalt-mediated radical polymerization
Debuigne, Antoine ULg; Schoumacher, Matthieu; Willet, Nicolas ULg et al

in Chemical Communications (2011), 47(47), 12703-12705

The photoinitiated cobalt-mediated radical polymerization enables the synthesis of novel alpha-functional and alpha,omega-telechelic polymers. In combination with ring-opening polymerization, it also ... [more ▼]

The photoinitiated cobalt-mediated radical polymerization enables the synthesis of novel alpha-functional and alpha,omega-telechelic polymers. In combination with ring-opening polymerization, it also produces new amphiphilic copolymers which self-assemble into flower-like vesicles in water. [less ▲]

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See detailPreparation and characterization of thermo-responsive gold nanohybrids
Liu, Ji ULg; Hurtgen, Marie ULg; Detrembleur, Christophe ULg et al

Poster (2011, October 25)

Stimuli-responsive nano-materials have been playing increasingly important roles in the biomedical field due to their ability to alter the physico-chemical properties in response to external stimuli, such ... [more ▼]

Stimuli-responsive nano-materials have been playing increasingly important roles in the biomedical field due to their ability to alter the physico-chemical properties in response to external stimuli, such as temperature, pH, ionic strength, magnetic field, etc. Nanohybrids bearing an inorganic core and thermo-responsive polymer shell are particularly applicable in target delivery and controlled drug release. Poly (N-vinylcaprolactam) (PNVCL) and its copolymers, exhibiting lower critical solution temperature (LCST) where the transition between hydrophilic and hydrophobic state happens, is one of the optimal choices for this core/shell structure. Here we present the in-situ fabrication of thermo-responsive gold nanohybrids coated with a novel poly(vinyl alcohol)-b-poly(N-vinylcaprolactam) (PVOH-b-PNVCL) block copolymer prepared by the cobalt-mediated radical polymerization (CMRP). The interaction between both PVOH and PNVCL segments and gold nanoparticles was confirmed by FT-IR spectra. A sharp thermo-induced phase transition with a good reversibility upon change in temperature was detected by DLS and UV/vis spectrometer. Furthermore, the presence of hydrophilic PVOH moieties endows the gold nanohybrids with improved colloidal stability above LCST without any flocculation detected, compared with the gold nanoparticles stabilized with PNVCL homopolymer. This kind of gold nanohybrids can be envisaged as a new drug delivery vehicle. [less ▲]

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See detailStealth macromolecular platforms for the design of MRI blood pool contrast agents
Grogna, Mathurin ULg; Cloots, Rudi ULg; Luxen, André ULg et al

in Polymer Chemistry (2011), 2(10), 2316-2327

Stealth macromolecular platforms bearing alkyne groups and poly(ethylene oxide) brushes were synthesized by reversible addition fragmentation chain transfer (RAFT) polymerization. The anchoring of Gd3 ... [more ▼]

Stealth macromolecular platforms bearing alkyne groups and poly(ethylene oxide) brushes were synthesized by reversible addition fragmentation chain transfer (RAFT) polymerization. The anchoring of Gd3+-chelates bearing an azide group was then carried out by the Huisgen 1,3-dipolar cycloaddition (“click”) reaction in mild conditions, leading to macrocontrast agents for MRI applications. The gadolinium complex is hidden in the PEO shell that renders the macrocontrast agents free of any cytotoxicity and stealth to proteins of the immune system. Relaxometry measurements have evidenced an improved relaxivity of the macrocontrast agent compared to ungrafted gadolinium chelate. Moreover, this relaxivity is further enhanced when the spacer length between the Gd3+-chelate and the polymer backbone is shorter, as the result of its decreased tumbling rate. These novel products are therefore promising candidates for MRI applications. [less ▲]

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See detailInfluence of nanoparticle-polymer interactions on the apparent migration behaviour of carbon nanotubes in an immiscible polymer blend
Tao, Fangfang; Nysten, Bernard; Baudouin, Anne-Christine et al

in Polymer (2011), 52(21), 4798-4805

We investigate the influence of nanoparticle–polymer interactions on the apparent migration behavior of multiwall carbon nanotubes (CNTs) in an immiscible polymer blend of ethylene-acrylate copolymer (EA ... [more ▼]

We investigate the influence of nanoparticle–polymer interactions on the apparent migration behavior of multiwall carbon nanotubes (CNTs) in an immiscible polymer blend of ethylene-acrylate copolymer (EA) and polyamide 12 (PA). The polymer-CNTs interaction is tuned by using different surface modification strategies, comprising grafting and coating. Poly(methyl methacrylate) (PMMA) and polystyrene (PS) are chosen as surface modifiers. The nanocomposite materials are prepared by melt-blending polymer-modified-CNTs in EA and PA. Polymer-grafted-CNTs tend to concentrate at the PA/EA interface, even if predispersed in PA, as opposed to pristine CNTs, which stay inside PA under the same circumstances. This new behavior is consistent with the morphology of PA/EA/(PMMA or PS) ternary blends and suggest a dominance of interfacial thermodynamics on CNTs localization. If we use polymer-coated-CNTs instead, the behavior depends on molar mass of the coating polymer. For low molar mass, it is similar to that of pristine CNTs and indicates desorption of the coating, owing to the weak interaction with the CNTs surface. Interestingly, we observe that long PS chains do not desorb and can drive the CNTs to the interface of the PA/EA blend. Moreover, the influence of kinetics is clearly observed through the dependence of CNTs interfacial confinement on dispersed droplet size. [less ▲]

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See detailMicrostructure characterisation of nanocomposite polymeric foams by X-ray microtomography
Plougonven, Erwan ULg; Marchot, Pierre ULg; Detrembleur, Christophe ULg et al

Poster (2011, September 21)

Recent advances in microstructured materials have given rise to many new types of composites that exhibit original and interesting physical properties. For example, a nanocomposite made of carbon ... [more ▼]

Recent advances in microstructured materials have given rise to many new types of composites that exhibit original and interesting physical properties. For example, a nanocomposite made of carbon nanotubes inside a polymer matrix shows exceptional electromagnetic interference shielding effectiveness when foamed. However, the effective properties of such materials strongly depend on the shape and topology of the microstructural cells. An accurate method for investigating the cellular microstructure is X-ray microtomography (XRµT), for it is non-destructive, and it provides 3D geometric information. Although it cannot be used to observe nanofiller dispersion, it has a strong potential for cell structure characterization. In order to reduce the need for trial and error for tailoring these materials, our objective is to characterize, using XRµT, two different types of foaming procedures, namely supercritical CO2 batch foaming and freeze drying. As the resolution is limited compared to cell size, we have developed a novel statistical method based on 3D autocorrelation to determine characteristic length and examine anisotropy. We present results for these two types of foams and show the limitations of this method. [less ▲]

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See detailGlucose-responsive layer-by-layer microcapsules as self-regulated insulin delivery system
Alaimo, David ULg; Detrembleur, Christophe ULg; Auzély-Velty, Rachel et al

Poster (2011, September 03)

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See detailConvenient grafting through approach for the preparation of stealth polymeric blood pool magnetic resonance imaging contrast agents
Grogna, Mathurin ULg; Cloots, Rudi ULg; Luxen, André ULg et al

in Journal of Polymer Science. Part A, Polymer Chemistry (2011), 49(17), 3700-3708

New hydrosoluble magnetic resonance imaging (MRI) macrocontrast agents are synthesized by reversible addition fragmentation chain transfer (RAFT) copolymerization of poly(ethylene oxide) methyl ether ... [more ▼]

New hydrosoluble magnetic resonance imaging (MRI) macrocontrast agents are synthesized by reversible addition fragmentation chain transfer (RAFT) copolymerization of poly(ethylene oxide) methyl ether acrylate (PEOMA) with an acrylamide bearing a ligand for gadolinium, followed by the complexation of Gd3+. This convenient and simple grafting through approach leads to macrocontrast agents with a high relaxivity at high frequency that is imparted by the restricted tumbling of the Gd3+ complex caused by its attachment to the polymer backbone. Importantly a very low protein adsorption is also evidenced by the hemolytic CH50 test. It is the result of the poly(ethylene oxide) (PEO) brush that efficiently hides the gadolinium complex and renders it stealth to the proteins of the immune system. Improved contrast and long blood circulating properties are thus expected for these macrocontrast agents. [less ▲]

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