References of "Jérôme, Christine"
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See detailDouble thermoresponsive di- and triblock copolymers based on N-vinylcaprolactam and N-vinylpyrrolidone: synthesis and comparative study of solution behaviour
Kermagoret, Anthony ULg; Mathieu, Kevin ULg; Thomassin, Jean-Michel ULg et al

in Polymer Chemistry (in press)

Poly(N-vinylcaprolactam) (PNVCL) and poly(N-vinylpyrrolidone) (PNVP) are water soluble polymers of interest especially in the biomedical field. Moreover, PNVCL is characterized by a lower critical ... [more ▼]

Poly(N-vinylcaprolactam) (PNVCL) and poly(N-vinylpyrrolidone) (PNVP) are water soluble polymers of interest especially in the biomedical field. Moreover, PNVCL is characterized by a lower critical solution temperature close to 36 °C in water, which makes it useful for the design of thermoresponsive systems. In this context, we used the cobalt-mediated radical polymerization (CMRP) and reaction coupling (CMRC) for synthesizing a series of well-defined NVCL and NVP-based copolymers, including statistical copolymers as well as double thermoresponsive diblocks and triblocks. Dynamic light scattering and turbidimetry analyses highlighted the crucial impact of the copolymer composition and architecture on the cloud point temperature (TCP) of each segment and also their influence on the multistep assembly behaviour of block copolymers. Addition of NaCl enabled us to adjust the inter-TCP range of the di- and triblock in which selective precipitation of one block and self-assembly of the copolymer were favoured. Overall, data presented here provide a basis for the synthesis of a broad range of NVCL/NVP based copolymer architectures with a tunable thermal response in water. [less ▲]

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See detailPolymer topology revealed by ion mobility coupled with mass spectrometry
Morsa, Denis ULg; Defize, Thomas ULg; Dehareng, Dominique ULg et al

in Analytical Chemistry (in press)

Hyperbranched and star shaped polymers have raised tremendous interests because of their unusual structural and photochemical properties which provide them potent applications in various domains, namely ... [more ▼]

Hyperbranched and star shaped polymers have raised tremendous interests because of their unusual structural and photochemical properties which provide them potent applications in various domains, namely in the biomedical field. In this context, the development of adequate tools aiming to probe particular three-dimensional features of such polymers is of crucial importance. In this present work, ion mobility coupled with mass spectrometry was used to experimentally derive structural information related to cationized linear and star-shaped poly-ε-caprolactones as a function of their charge state and chain length. Two major conformations were observed and identified using theoretical modeling: (1) near spherical conformations whose size is invariant with the polymer topology for long and lightly charged chains and (2) elongated conformations whose size varies with the polymer topology for short and highly charged chains. These conformations were further confirmed by collisional activation experiments based on the ejection thresholds of the coordinated cations that vary according to the elongation amplitude of the polymer chains. Finally, a comparison between solution and gas-phase conformations highlights a compaction of the structure with a loss of specific chain arrangements during the ionization and desolvation steps of the electrospray process, fueling the long-time debated question related to the preservation of the analyte structure during the transfer into the mass spectrometer. [less ▲]

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See detailIn situ bidentate to tetradentate ligand exchange reaction in cobalt-mediated radical polymerization
Kermagoret, Anthony ULg; Jérôme, Christine ULg; Detrembleur, Christophe ULg et al

in European Polymer Journal (in press)

Organometallic-mediated radical polymerization (OMRP) has seen a significant growth in the last years notably due to the development of new metal complexes, especially cobalt derivatives. Despite of this ... [more ▼]

Organometallic-mediated radical polymerization (OMRP) has seen a significant growth in the last years notably due to the development of new metal complexes, especially cobalt derivatives. Despite of this, none of the reported complexes offers optimal control for monomers with very different reactivity, which somewhat limits the synthesis of copolymers. In order to expand the scope of cobalt-mediated radical polymerization (CMRP), we investigated an in situ ligand exchange reaction for modulating the properties of the cobalt complex at the polymer chain-end and adjusting the C-Co bond strength involved in the control process. With the aim of improving the synthesis of poly(vinyl acetate)-b-poly(n-butyl acrylate) copolymers, bidentate acetylacetonate ligands, which impart high level of control to the polymerization of vinyl acetate (VAc), were replaced in situ at the PVAc-cobalt chain-end by tetradentate Salen type ligands that are more suited to acrylates. [less ▲]

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See detailInput of supercritical carbon dioxide to polymer synthesis: an overview
Boyère, Cédric; Jérôme, Christine ULg; Debuigne, Antoine ULg

in European Polymer Journal (in press)

The ongoing search for environmentally friendlier alternative to the organic solvents used in chemical processes has led to the development of technologies based on supercritical carbon dioxide (scCO2 ... [more ▼]

The ongoing search for environmentally friendlier alternative to the organic solvents used in chemical processes has led to the development of technologies based on supercritical carbon dioxide (scCO2), which is non-flammable, non-toxic and relatively inert fluid. Polymer chemistry does not escape this trend and last achievements in the field of polymer synthesis in scCO2 are reviewed here. Without claiming to be exhaustive, we go through and discuss the benefits of the main polymerization processes in scCO2 including homogeneous, precipitation, dispersion, suspension and emulsion systems. A particular attention is drawn to water/carbon dioxide emulsion polymerization and to the suited surface active agents. This review also underlines that heterogeneous polymerization based on CO2 is more than a strategy for reducing the ecological footprint of the polymer production but it allows structuring the polymer materials into particles or highly interconnected macroporous networks. [less ▲]

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See detailDevelopment of functionalized nanoparticles for vaccine delivery to dendritic cells: a mechanistic approach
Silva, Joana M.; Vandermeulen, Gaëlle; Oliveira, Vanessa G. et al

in Nanomedicine (in press)

Aim: Produce biodegradable nanoparticles to target antigen-presenting cells and evaluate their potential to be used as a vaccine delivery system. Materials & methods: Untargeted PEGylated PLGA-based ... [more ▼]

Aim: Produce biodegradable nanoparticles to target antigen-presenting cells and evaluate their potential to be used as a vaccine delivery system. Materials & methods: Untargeted PEGylated PLGA-based nanoparticles and mannose-grafted nanoparticles were formulated and physicochemically characterized. Immortalized and primary antigen-presenting cells were used to study nanoparticle internalization patterns. The endocytic pathways and intracellular trafficking followed by nanoparticles were also investigated. Results & discussion: Nanoparticles displayed mannose residues available for binding at the nanoparticle surface. Different nanoparticle internalization patterns by immortalized and primary antigen presenting cells were verified. Macropinocytosis, clathrin-mediated endocytosis, caveolin- and lipid raft-dependent endocytosis are involved in nanoparticles internalization. Nanoparticles demonstrate both endo-lysosomal and cytosolic localizations and a tendency to accumulate nearby the endoplasmic reticulum. Conclusion & future perspective: The developed nanoparticles might drive antigens to be presented through MHC class I and II molecules to both CD8+ and CD4+ T cells, favoring a complete and coordinated immune response. [less ▲]

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See detailBlock, random and palm-tree amphiphilic fluorinated copolymers: controlled synthesis, surface activity and use as dispersion polymerization stabilizers
Alaimo, David ULg; Beigbeder, Alexandre; Dubois, Philippe et al

in Polymer Chemistry (2014), 5(18), 5273-5282

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See detailThermo-responsive gold/poly(vinyl alcohol)-b-poly(N-vinylcaprolactam) core–corona nanoparticles as a drug delivery system
Liu, Ji ULg; Detrembleur, Christophe ULg; Hurtgen, Marie et al

in Polymer Chemistry (2014), 5(18), 5289-5299

Core–corona gold/poly(vinyl alcohol)-b-poly(N-vinylcaprolactam) nanoparticles (gold@PVOH-b-PNVCL NPs) were fabricated via an in situ method, where a gold salt was reduced within the macromolecular aqueous ... [more ▼]

Core–corona gold/poly(vinyl alcohol)-b-poly(N-vinylcaprolactam) nanoparticles (gold@PVOH-b-PNVCL NPs) were fabricated via an in situ method, where a gold salt was reduced within the macromolecular aqueous solution. Arrangement of macromolecular chains on the surface of gold cores was studied by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy and infrared spectroscopy. The responsiveness to temperature and the preserved colloidal stability of the gold@PVOH-b-PNVCL NPs above the lower critical solution temperature (LCST) were confirmed by dynamic light scattering and turbidity measurements. The drug loading capacity (DLC of ca. 1.3–2.8 wt%) of the gold@PVOH-b-PNVCL NPs as a drug delivery system (DDS) was tested with Nadolol®, a hydrophilic drug, and the release behaviours were studied at several temperatures. PVOH-b-PNVCL copolymers with an LCST of a few degrees above the biological temperature (37 °C), for example, PVOH180-b-PNVCL110 (LCST of 41 °C), are preferential, due to the slower release at 37 °C, but a faster release at temperatures that are a few degrees higher. The cytocompatibility of the gold@PVOH-b-PNVCL NPs against mouse fibroblastic L929 cells was evaluated via the MTS assay. Cellular uptake within MEL-5 human melanoma cells was studied by confocal laser scanning microscopy, fluorescence-activated cell sorting and TEM techniques and it showed that gold@PVOH-b-PNVCL NPs preferably accumulated within the cellular cytoplasm, with an incubation concentration and period-dependent uptake process. All these results corroborated a general utility of these thermo-responsive gold@PVOH-b-PNVCL NPs for drug delivery and controlled drug release. [less ▲]

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See detailSynthesis of well-defined ethylene-based copolymers: on track using organometallic-mediated radical polymerization
Debuigne, Antoine ULg; Kermagoret, Anthony ULg; Jérôme, Christine ULg et al

Conference (2014, September 19)

Organometallic-Mediated Radical Polymerization (OMRP)1 has received renewed interest in recent years since proving its efficiency for non-activated monomers like vinylacetate (VAc), N-vinylamides, etc ... [more ▼]

Organometallic-Mediated Radical Polymerization (OMRP)1 has received renewed interest in recent years since proving its efficiency for non-activated monomers like vinylacetate (VAc), N-vinylamides, etc. Nevertheless, important mechanistic questions and challenges remained. A major goal in the field of controlled radical polymerization today consists in the design of well-defined ethylene containing (co)polymers. A recent mechanistic study on the impact of head-to-head addition on the course of the VAc polymerization by OMRP provided a strong incentive to evaluate the copolymerization of VAc with ethylene by this technique. Indeed, the latter revealed that dormant chains resulting from inverted head-to-head additions in the VAc polymerization, which mimics a terminal ethylene-cobalt moiety, reactivates at a similar rate compared to the ones resulting from the regular head-to-tail addition. As a result, well-defined statistical and block-like ethylene-based copolymers were prepared. These achievements represent an important step towards a versatile synthetic platform for polyolefine-based materials. [less ▲]

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See detailThiophene derivatives with donor–π–acceptor structures for enhanced light-absorption properties and efficient cationic polymerization upon green-light irradiation
Telitel, Sofia; Ouhib, Farid ULg; Fouassier, Jean-Pierre et al

in Macromolecular Chemistry and Physics (2014), 215(16), 1514-1524

Positively charged thermoresponsive nanogels (NGs) are easily synthesized by precipitation polymerization of N-isopropyl­acrylamide and 2-dimethyl(aminoethyl)­methacrylate crosslinked with dendritic ... [more ▼]

Positively charged thermoresponsive nanogels (NGs) are easily synthesized by precipitation polymerization of N-isopropyl­acrylamide and 2-dimethyl(aminoethyl)­methacrylate crosslinked with dendritic polyglycerol. The NGs are characterized in terms of size, thermoresponsive properties, and Z potential. Their potential applications as drug delivery carriers are evaluated by the encapsulation and release of different anticancer drugs. As model drugs, doxorubicin and methotrexate are studied. [less ▲]

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See detailSupercritical CO2, impregnation to prepare drug-loaded implants: inpregantion of anti-inflammatory drugs into sutures
Champeau, Mathilde; Tassaing, Thierry; Thomassin, Jean-Michel ULg et al

Conference (2014, July 10)

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See detailSynthesis of degradable polyphosphoester copolymers for templating calcium carbonate drug delivery carriers
Ergül, Zeynep ULg; Debuigne, Antoine ULg; Calvignac, Brice et al

Conference (2014, July 09)

Degradable acid bearing polyphosphoester (PPE) copolymers were prepared by combination of organocatalyzed ring opening polymerization and click chemistry. Their solution behavior and ability to complex ... [more ▼]

Degradable acid bearing polyphosphoester (PPE) copolymers were prepared by combination of organocatalyzed ring opening polymerization and click chemistry. Their solution behavior and ability to complex calcium ions were studied as well as their capacity to template CaCO3 particles dedicated to drug delivery. [less ▲]

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See detailCollapsing and reswelling kinetics of thermoresponsive polymers on surfaces: a matter of confinement and constraints
Willet, Nicolas ULg; Gabriel, Sabine ULg; Jérôme, Christine ULg et al

in Soft Matter (2014), 10

We report on the collapsing and reswelling ability of grafted poly(methyl vinyl ether) chains of different molecular architectures. In order to study the influence of constraints and confinement of the ... [more ▼]

We report on the collapsing and reswelling ability of grafted poly(methyl vinyl ether) chains of different molecular architectures. In order to study the influence of constraints and confinement of the chains, the polymer was grafted onto AFM tips, as a model of a curved nano-sized surface, and onto macroscopic silicon substrates for comparison purposes. AFM-based force spectroscopy experiments were performed to characterise at the nanoscale the temperature-dependent collapsing process and the reversibility to the swollen state on both substrates. The reversible character of the thermoresponsive transition and its kinetics were shown to greatly depend on the polymer architecture and the constraints encountered by the chains. [less ▲]

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See detailIn situ FTIR micro-spectroscopy to investigate polymeric fibers under supercritical carbon dioxide: CO2 sorption and swelling measurements
Champeau, Mathilde; Thomassin, Jean-Michel ULg; Jérôme, Christine ULg et al

in Journal of Supercritical Fluids (2014), 90

An original experimental set-up combining a FTIR (Fourier Transformed InfraRed) microscope with a high pressure cell has been built in order to analyze in situ and simultaneously the CO2 sorption and the ... [more ▼]

An original experimental set-up combining a FTIR (Fourier Transformed InfraRed) microscope with a high pressure cell has been built in order to analyze in situ and simultaneously the CO2 sorption and the polymer swelling of microscopic polymer samples, such as fibers, subjected to supercritical carbon dioxide. Thanks to this experimental set-up, we have determined as a function of the CO2 pressure (from 2 to 15 MPa) the CO2 sorption and the polymer swelling at T = 40 °C of four polymer samples, namely PEO (polyethylene oxide), PLLA (poly-l-lactide acid), PET (polyethylene terephtalate) and PP (polypropylene). The quantity of CO2 sorbed in all the studied polymers increases with pressure. PEO and PLLA display a significant level of CO2 sorption (20 and 25% respectively, at P = 15 MPa). However, we observe that a lower quantity of CO2 can be sorbed into PP and PET (7 and 8% respectively, at P = 15 MPa). Comparing their thermodynamic behaviors and their intrinsic properties, we emphasize that a high CO2 sorption can be reach if on one hand, the polymer is able to form specific interaction with CO2 in order to thermodynamically favor the presence of CO2 molecules inside the polymer and on the other, displays high chains mobility in the amorphous region. PLLA and PEO fulfilled these two requirements whereas only one property is fulfilled by PET (specific interaction with CO2) and PP (high chains mobility). Finally, we have found that for a given CO2 sorption, the resulting swelling of the polymer depends mainly on its crystallinity. [less ▲]

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See detailSynthesis of hybrid nanoparticles for theranostics
Liu, Ji ULg; Detrembleur, Christophe ULg; Duguet, Etienne et al

Conference (2014, May 28)

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See detailSynthesis of a glucosamine labeled amphiphilic polymer for drug delivery application
Riva, Raphaël ULg; Boyère, Cédric; Debuigne, Antoine ULg et al

Poster (2014, May 27)

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See detailMultilayered chitosan-based fibers for skin regenaration applications
Croisier, Florence ULg; Detrembleur, Christophe ULg; Jérôme, Christine ULg

Poster (2014, May 26)

Chitosan is a natural polymer derived from the chitin of crustacean or mushroom shells, that intrinsically presents haemostatic, mucoadhesive, antimicrobial and immunostimulant properties. This ... [more ▼]

Chitosan is a natural polymer derived from the chitin of crustacean or mushroom shells, that intrinsically presents haemostatic, mucoadhesive, antimicrobial and immunostimulant properties. This polysaccharide has shown a great potential for biomedical and pharmaceutical applications, on account of its remarkable compatibility with physiological medium. Besides, it is degraded in a physiological environment into non-toxic products, which make chitosan an outstanding candidate for short- to medium-term applications. 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). This technique uses a high voltage to create an electrically charged jet of polymer solution or melt which leads to fibers formation. Depending on the polymer characteristics (a.o. molecular weight, solution viscosity and conductivity) and processing conditions (electric potential, distance between syringe-capillary and collection plate, concentration, flow rate), polymer fibers ranging from nanometers to a few microns in diameter can be obtained and subsequently used as potential 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. The antibacterial properties of the obtained material were then assessed, and the presence of a multilayered deposit was confirmed by several techniques. The multilayered chitosan-based nanofibers produced present great prospects for the preparation of new biomedical scaffolds - such as wound dressings that could improve skin regeneration. [less ▲]

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See detailElectrografting of polythiophenes on zinc oxide nanorods for photovoltaic cells
Demarteau, Jérémy ULg; Ouhib, Farid ULg; Henrist, Catherine ULg et al

Poster (2014, May 20)

As the rarefaction of fossil energies, photovoltaic cells are certainly amongst the most important energy sources for the future. Our work concentrated on hybrid photovoltaic cells that are based on ... [more ▼]

As the rarefaction of fossil energies, photovoltaic cells are certainly amongst the most important energy sources for the future. Our work concentrated on hybrid photovoltaic cells that are based on organic (polythiophene) and inorganic components (ZnO nanorods). The technology that maximizes the contact area between the two semi-conductor n and p while maintaining two separate components is the interdigital configuration. As the inorganic part, perfectly well aligned zinc oxide (ZnO) 1D nanostructures have been synthesized by hydrothermal growth on ZnO-seeded FTO substrates. SEM, AFM and XRD characterizations evidence patterned well- aligned nanorods with high c-axis, their roughness of surface and the length of their nanostructure. Concerning the organic component, we synthetize polythiophenes based diblock copolymer with high degree of regioregularity and predetermined molecular weight using Grignard Methatis (GRIM) process. Diblock polythiophene based copolymers are of interest because of the possibility of generating multifunctional materials (by associating the specific properties of each block), including their ability for self-assembly into well-defined nanostructures (fibrils or micelles) with controllable dimensions. Poly(3-hexylthiophene) (P3HT) composes the first block and the second block is either a polythiophene bearing an acrylate group on each monomer unit (PAcET), or a polythiophene bearing both acrylate and poly(ethylene glycol) side chains (P(AcET-co-PEGET)). Typically, the acrylates are used to fixe in a covalent way the copolymer to ZnO nanorods, while the PEG grafts are necessary for the solubilisation of the copolymer in the electrografting medium. 1H NMR and DLS characterizations allow us to find the backbone and the micellar structure of the copolymer. Cathodic polarization (electrografting) of ZnO nanorods induces electropolymerization of acrylate groups, leading to an adherent organized film of poly(thiophene)-based micelles. During the illumination tests, we obtained a typical response of a photovoltaic despite the low yields. This promising synthetic route opens exciting perspectives for the production and the electrochemical functionalization of different lengths of ZnO nanowires, which seems to be promising candidate for hybrids photovoltaic cells. [less ▲]

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