References of "Detrembleur, Christophe"
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See detailPoly(vinyl ester 1,2,3-triazolium)s: a new member of the poly(ionic liquid)s family
Obadia, M. M.; Colliat-Dangus, G.; Debuigne, Antoine ULg et al

in Chemical Communications (in press)

A vinyl ester monomer carrying a pendant 1,2,3-triazole group is synthesized in two steps and polymerized by cobalt-mediated radical polymerization. Subsequent alkylation with N-methyl bis ... [more ▼]

A vinyl ester monomer carrying a pendant 1,2,3-triazole group is synthesized in two steps and polymerized by cobalt-mediated radical polymerization. Subsequent alkylation with N-methyl bis[(trifluoromethyl)sulfonyl]imide affords the corresponding poly(vinyl ester 1,2,3-triazolium). This unprecedented example of poly(vinyl ester ionic liquid) exhibits an ionic conductivity of 9.2 × 10(-7) S cm(-1) at 30 °C [less ▲]

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See detailGold nanorods coated with mesoporous silica shell as drug delivery system for remote near infrared light-activated release and potential phototherapy
Liu, Ji; Detrembleur, Christophe ULg; De Pauw-Gillet, Marie-Claire ULg et al

in Small (Weinheim an der Bergstrasse, Germany) (in press)

In this study, we report the synthesis of a nanoscaled drug delivery system, which is composed of a gold nanorod-like core and a mesoporous silica shell (GNR@MSNP) and partially uploaded with phase ... [more ▼]

In this study, we report the synthesis of a nanoscaled drug delivery system, which is composed of a gold nanorod-like core and a mesoporous silica shell (GNR@MSNP) and partially uploaded with phase-changing molecules (1-tetradecanol, TD, Tm 39 degrees C) as gatekeepers, as well as its ability to regulate the release of doxorubicin (DOX). Indeed, a nearly zero premature release is evidenced at physiological temperature (37 degrees C), whereas the DOX release is efficiently achieved at higher temperature not only upon external heating, but also via internal heating generated by the GNR core under near infrared irradiation. When tagged with folate moieties, GNR@MSNPs target specifically to KB cells, which are known to overexpress the folate receptors. Such a precise control over drug release, combining with the photothermal effect of GNR cores, provides promising opportunity for localized synergistic photothermal ablation and chemotherapy. Moreover, the performance in killing the targeted cancer cells is more efficient compared with the single phototherapeutic modality of GNR@MSNPs. This versatile combination of local heating, phototherapeutics, chemotherapeutics and gating components opens up the possibilities for designing multifunctional drug delivery systems. [less ▲]

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See detailSelf-assembly of a triblock terpolymer mediated by hydrogen-bonded complexes
Guerlain, Claire; Piogé, Sandie; Detrembleur, Christophe ULg et al

in Journal of Polymer Science. Part A, Polymer Chemistry (2015), 53(3), 459-467

A poly(methyl methacrylate)-block-poly(4-vinylpyridine)-block-polystyrene (PMMA-b-P4VP-b-PS) triblock terpolymer is synthesized by ATRP to study its self-assembly with PAA in organic solvents. The self ... [more ▼]

A poly(methyl methacrylate)-block-poly(4-vinylpyridine)-block-polystyrene (PMMA-b-P4VP-b-PS) triblock terpolymer is synthesized by ATRP to study its self-assembly with PAA in organic solvents. The self-assembly behavior of this system is compared with the one of a mixture of two diblocks, namely polystyrene-block-poly(4-vinylpyridine) (PS-b-P4VP) and poly(methyl methacrylate)-block-poly(methacrylic acid) (PMMA-b-PMAA). For both systems, formation of hydrogen-bonded complexes between the P4VP and PMAA or PAA blocks occurs. These complexes become insoluble in the solvent used and micelles with a P4VP/P(M)AA complexes core surrounded by PS and PMMA coronal chains are obtained in both cases. These micelles are analyzed by DLS and TEM. Spherical micelles are formed for both systems but the hydrodynamic radii obtained for the two types of micelles are different. Indeed, the micelles formed by the PMMA-b-P4VP-b-PS + PAA system are smaller than those observed for the PS-b-P4VP + PMMA-b-PMAA system. Finally, the effect of the molar ratio of the P4VP/PMAA complexing blocks is investigated. [less ▲]

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See detailStimuli-responsive behavior of micelles prepared from a poly(vinyl alcohol)-block-poly(acrylic acid)-block-poly(4-vinylpyridine) triblock terpolymer
Poggi, Elio; Guerlain, Claire; Debuigne, Antoine ULg et al

in European Polymer Journal (2015), 62

A poly(vinyl alcohol)-block-poly(acrylic acid)-block-poly(4-vinylpyridine) triblock terpolymer (PVOH-b-PAA-b-P4VP) is prepared by hydrolyzing a poly(vinyl acetate)-block-poly(acrylonitrile)-block-poly(4 ... [more ▼]

A poly(vinyl alcohol)-block-poly(acrylic acid)-block-poly(4-vinylpyridine) triblock terpolymer (PVOH-b-PAA-b-P4VP) is prepared by hydrolyzing a poly(vinyl acetate)-block-poly(acrylonitrile)-block-poly(4-vinylpyridine) precursor (PVAc-b-PAN-b-P4VP) synthesized by a combination of cobalt-mediated radical polymerization (CMRP) and nitroxide mediated polymerization (NMP). The PVOH-b-PAA-b-P4VP terpolymer is further micellized in water and the accordingly obtained micellar structures are characterized by a combination of dynamic light scattering (DLS) and cryo-transmission electron microscopy (cryo-TEM) as a function of pH. Well-defined micelles are observed in the whole pH range except for pH values below 4.5 where non-aggregated chains (unimers) are present. The formation of micelles can be rationalized by the formation of insoluble PAA/P4VP inter-polyelectrolyte complexes in the 4.5–6 pH range while hydrophobic P4VP cores are observed at pH values above 6. Finally, the effect of the addition of different salts on the micellar characteristic features is investigated. [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 (2015), 62

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 detailDirect route to well-defined poly(ionic liquid)s by controlled radical polymerization in water
Cordella, Daniela ULg; Kermagoret, Anthony ULg; Debuigne, Antoine ULg et al

in ACS Macro Letters (2014), 3

The precision synthesis of poly(ionic liquid)s (PILs) in water is achieved for the first time by the cobalt-mediated radical polymerization (CMRP) of N-vinyl-3-alkylimidazolium-type monomers following two ... [more ▼]

The precision synthesis of poly(ionic liquid)s (PILs) in water is achieved for the first time by the cobalt-mediated radical polymerization (CMRP) of N-vinyl-3-alkylimidazolium-type monomers following two distinct protocols. The first involves the CMRP of various 1-vinyl-3-alkylimidazolium bromides conducted in water in the presence of an alkyl–cobalt(III) complex acting as a monocomponent initiator and mediating agent. Excellent control over molar mass and dispersity is achieved at 30 °C. Polymerizations are complete in a few hours, and PIL chain-end fidelity is demonstrated up to high monomer conversions. The second route uses the commercially available bis(acetylacetonato)cobalt(II) (Co(acac)2) in conjunction with a simple hydroperoxide initiator (tert-butyl hydroperoxide) at 30, 40, and 50 °C in water, facilitating the scaling-up of the technology. Both routes prove robust and straightforward, opening new perspectives onto the tailored synthesis of PILs under mild experimental conditions in water. [less ▲]

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See detailPoly( N-vinylcaprolactam): A thermoresponsive macromolecule with promising future in biomedical field
Liu, Ji; Debuigne, Antoine ULg; Detrembleur, Christophe ULg et al

in Advanced Healthcare Materials (2014), 3(12), 1941-1968

Poly( N -vinylcaprolactam) (PNVCL) is a thermoresponsive and biocompatible polymer that raises an increasing interest in the biomedical area, especially in drug delivery systems (DDS) that include ... [more ▼]

Poly( N -vinylcaprolactam) (PNVCL) is a thermoresponsive and biocompatible polymer that raises an increasing interest in the biomedical area, especially in drug delivery systems (DDS) that include micelles, hydrogels, and hybrid particles. The thermoresponsiveness of PNVCL, used alone or in combination with other stimuli- responsive polymers or particles (pH, magnetic fi eld, or chemicals), is often key in the loading and/or release process in these DDS. The renewed focus on this polymer, which is known for decades, is to a large extent due to recent progress in synthetic strategies. Especially, the advent of efficient controlled radical polymerization (CRP) methods for NVCL monomer gives now access to unprecedented well-defi ned NVCL-based copolymers with unique properties. This Review article addresses up-to-date synthetic aspects, biological features, and biomedical applications of the latest NVCL-containing systems. [less ▲]

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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 (2014), 5(22), 6534-6544

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 detailA facile and fast electrochemical route to produce functional few-layer graphene sheets for lithium battery anode application
Ouhib, Farid ULg; Aqil, Abdelhafid ULg; Thomassin, Jean-Michel ULg et al

in Journal of Materials Chemistry A (2014), 2(37), 15298-15302

A simple approach for the production of polymer functionalized graphene nanosheets is reported. The resulting polyacrylonitrile chemisorbed on graphene sheets is made of 1 to 2 layers, with a large ... [more ▼]

A simple approach for the production of polymer functionalized graphene nanosheets is reported. The resulting polyacrylonitrile chemisorbed on graphene sheets is made of 1 to 2 layers, with a large majority of graphene single-layers. This novel functionalized graphene exhibits good cycling stability as an anode in Li-ion batteries without a conductive additive or binder. [less ▲]

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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 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 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 detailChemical fixation of CO2 with epoxides: towards the synthesis of cyclic carbonates, precursors of CO2-based polyurethanes
Gennen, Sandro ULg; Grignard, Bruno ULg; Gilbert, Bernard ULg et al

Poster (2014, May 20)

Due to concerns about global warming combined with the decrease of fossil resources, the chemical transformation of carbon dioxide into added-value products has gained interest in both academic and ... [more ▼]

Due to concerns about global warming combined with the decrease of fossil resources, the chemical transformation of carbon dioxide into added-value products has gained interest in both academic and industrial fields. To date, the chemical fixation of CO2 onto epoxides is one of the most promising ways to valorize carbon dioxide at an industrial scale . Indeed, cyclic carbonates are useful intermediates for polycarbonates and polyurethanes synthesis or can be used as electrolytes in lithium ion batteries. Although fixation of carbon dioxide onto epoxides has been extensively studied, the design of highly effective catalysts still remains a challenge. Here, we present a new highly efficient biocomponent organocatalyst based on the use of an ammonium salt (TBAI) in combination with single or double hydrogen bond donors activators (typically fluorinated alcohols). [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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