References of "Detrembleur, Christophe"
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See detailElectrografting onto ITO substrates of poly(thiophene)-based micelles decorated by acrylate groups
Ouhib, Farid ULg; Desbief, Simon; Lazzaroni, Roberto et al

in Polymer Chemistry (2013), 4(15), 4151-4161

We report on a simple process for the chemisorption of poly(thiophene)-based block copolymers onto ITO substrates. Two poly(thiophene) block copolymers functionalized by acrylates on the second block are ... [more ▼]

We report on a simple process for the chemisorption of poly(thiophene)-based block copolymers onto ITO substrates. Two poly(thiophene) block copolymers functionalized by acrylates on the second block are prepared by the Grignard Metathesis (GRIM) process. The first block is composed of poly(3-hexylthiophene) (P3HT) 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)). After characterizing their macromolecular parameters and optical properties, we investigate their ability to self-assemble into micelles in DMF solutions. This solvent is required for the electrografting procedure that is used for strongly anchoring the polymer to ITO. These micelles are expected to be formed by a P3HT core and a PAcET or P(AcET-co-PEGET) shell. When PEG side chains are present in the second block, the copolymer nicely self-assembles into micelles decorated by acrylates. Cathodic polarization of ITO induces chemisorption and polymerization of acrylate groups, leading to an adherent organized film of poly(thiophene)-based micelles. The optical absorption spectra show that the electrografted polymer chains have a degree of π-electron conjugation similar to that of crystalline P3HT films. In the absence of the PEG chains, the copolymer does not organize into micelles, due to the low stabilizing ability of the second block in DMF. [less ▲]

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See detailPolymer/carbon based composites as electromagnetic interference (EMI) shielding materials
Thomassin, Jean-Michel ULg; Jérôme, Christine ULg; Pardoen, Thomas et al

in Materials Science & Engineering : R (2013), 74(7), 211-232

The extensive development of electronic systems and telecommunications has lead to major concerns regarding electromagnetic pollution. Motivated by environmental questions and by a wide variety of ... [more ▼]

The extensive development of electronic systems and telecommunications has lead to major concerns regarding electromagnetic pollution. Motivated by environmental questions and by a wide variety of applications, the quest for materials with high efficiency to mitigate electromagnetic interferences (EMI) pollution has become a mainstream field of research. This paper reviews the state-of-the-art research in the design and characterization of polymer/carbon based composites as EMI shielding materials. After a brief introduction, in Section 1, the electromagnetic theory will be briefly discussed in Section 2 setting the foundations of the strategies to be employed to design efficient EMI shielding materials. These materials will be classified in the next section by the type of carbon fillers, involving carbon black, carbon fiber, carbon nanotubes and graphene. The importance of the dispersion method into the polymer matrix (melt-blending, solution processing, etc.) on the final material properties will be discussed. The combination of carbon fillers with other constituents such as metallic nanoparticles or conductive polymers will be the topic of Section 4. The final section will address advanced complex architectures that are currently studied to improve the performances of EMI materials and, in some cases, to impart additional properties such as thermal management and mechanical resistance. In all these studies, we will discuss the efficiency of the composites/devices to absorb and/or reflect the EMI radiation. [less ▲]

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See detailDesign of well-defined N-vinylamides based copolymers via organometalllic-mediated radical polymerization
Debuigne, Antoine ULg; Kermagoret, Anthony ULg; Fustin, Charles-André et al

Conference (2013, June 19)

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See detailEffect of head-to-head addition in vinyl acetate controlled radical polymerization: why is Co(acac)2-mediated polymerization so much better?
Morin, Aurélie N.; Detrembleur, Christophe ULg; Jérôme, Christine ULg et al

in Macromolecules (2013), 46(11), 4303-4312

The controlled polymerization of vinyl acetate has been recently achieved by several techniques, but PVAc with targeted Mn and low dispersity up to very high monomer conversions and high degrees of ... [more ▼]

The controlled polymerization of vinyl acetate has been recently achieved by several techniques, but PVAc with targeted Mn and low dispersity up to very high monomer conversions and high degrees of polymerization was only obtained with Co(acac)2 as controlling agent in the so-called CMRP, a type of organometallic mediated radical polymerization (OMRP). Other techniques (including ATRP, ITP, TERP, and RAFT/MADIX) have shown a more or less pronounced slowdown in the polymerization kinetics, which was attributed to the higher strength of the C−X bond between the radical PVAc chain and the trapping agent (X) in the dormant species and to a consequent slower reactivation after a less frequent head-to-head monomer addition. The reason for the CMRP exception is clarified by the present contribution. First, a detailed investigation by 1H, 13C and multiplicity-edited HSQC and DEPT-135 NMR of the PVAc obtained by CMRP, in comparison with a regular polymer made by free radical polymerization under the same conditions, has revealed that Co(acac)2 does not significantly alter the fraction of head-to-head sequences in the polymer backbone and that there is no accumulation of Co(acac)2-capped chains with a head-to-head ω end. Hence, both dormant chains (following the head-to-head and the head-to-tail monomer additions) must be reactivated at similar rates. A DFT study shows that this is possible because the dormant chains are stabilized not only by the C−Co σ bond but also by formation of a chelate ring through coordination of the ω monomer carbonyl group. The head-to-head dormant chain contains an inherently stronger C−Co bond but forms a weaker 6-membered chelate ring, whereas the weaker C−Co bond in the head-to-tail dormant chain is compensated by a stronger 5-membered chelate ring. Combination of the two effects leads to similar activation enthalpies, as verified by DFT calculations using a variety of local, gradient-corrected, hybrid and “ad hoc” functionals (BPW91, B3PW91, BPW91*, M06 and M06L). While the BDE(C−X) of model H-VAc−X molecules [X = Cl, I, MeTe, EtOC(S)S and Co(acac)2] are functional dependent, the BDE difference between head-to-head and head-to-tail dormant chain models is almost functional insensitive, with values of 5−9 kcal/mol for the ATRP, ITP and TERP models, 3−6 for the RAFT/MADIX model, and around zero for CMRP. [less ▲]

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See detailThe influence of foam morphology of multi-walled carbon nanotubes/poly(methyl methacrylate) nanocomposites on electrical conductivity
Tran, Minh Phuong ULg; Detrembleur, Christophe ULg; Alexandre, Michaël ULg et al

in Polymer (2013), 54(13), 3261-3270

Polymer/multi-walled carbon nanotubes (PMMA/MWNTs) nanocomposites foams are widely investigated during the last decade thanks to their potential applications as electromagnetic interferences shielding ... [more ▼]

Polymer/multi-walled carbon nanotubes (PMMA/MWNTs) nanocomposites foams are widely investigated during the last decade thanks to their potential applications as electromagnetic interferences shielding (EMI) materials. Electrical conductivity of the nanocomposite is a key parameter for these applications. In the frame of this work, we aim at establishing relationships between the foams morphology and their electrical conductivity. We therefore first design nanocomposite foams of various morphologies using supercritical carbon dioxide (scCO2) as physical foaming agent. The nanocomposites based on poly(methyl methacrylate) (PMMA) and different carbon nanotubes loadings are prepared by melt-mixing and foamed by scCO2 in various conditions of pressure, temperature and soaking time. The influence of these foaming conditions on the morphology of the foams (volume expansion, pore size, cell density, cell-wall thickness) is discussed. After measuring the electrical conductivity of the foams, we establish structure/properties relationships that are essential for further optimizations of the materials for the targeted application. [less ▲]

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See detailOne-pot controlled synthesis of double thermoresponsive N-vinylcaprolactam-based copolymers with tunable LCSTs
Kermagoret, Anthony ULg; Fustin, Charles-André; Bourguignon, Maxime et al

in Polymer Chemistry (2013), 4(8), 2575-2583

N-Vinylcaprolactam (NVCL) was copolymerized statistically for the first time in a controlled manner with hydrophilic N-vinylamide or hydrophobic vinylester monomers in order to precisely tune up and down ... [more ▼]

N-Vinylcaprolactam (NVCL) was copolymerized statistically for the first time in a controlled manner with hydrophilic N-vinylamide or hydrophobic vinylester monomers in order to precisely tune up and down the lower critical solution temperature (LCST) of the resulting copolymers. The incorporation of these segments in complex architectures was also considered. Several narrowly distributed NVCL-based copolymers were prepared by cobalt-mediated radical polymerization (CMRP) using the bis-(acetylacetonato)cobalt(II) complex as a controlling agent and N-methyl-N-vinylacetamide (NMVA), N-vinylacetamide (NVA), vinyl acetate (VAc) or vinyl pivalate (VPi) as comonomers. PNVCL-containing block copolymers having two discrete LCSTs were also synthesized following a one-pot strategy based on the sequential CMRP of NVCL followed by the copolymerization of NMVA with the residual NVCL. Upon gradual heating of aqueous solutions of such double thermoresponsive copolymers, we noticed a transition from free chains to micelles before full dehydration and collapse of the block copolymers. These advances represent a significant step towards the development of a platform based on thermoresponsive PNVCL copolymers with a single phase separation or multistep assembly behaviors. [less ▲]

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See detailIn situ nitroxide-mediated polymerization of styrene promoted by the N-tert-butyl-alpha-isopropylnitrone/BPO pair: ESR investigations
Detrembleur, Christophe ULg; Clément, Jean-Louis; Sciannaméa, Valérie et al

in Journal of Polymer Science. Part A, Polymer Chemistry (2013), 51(8), 1786-1795

The styrene polymerization initiated by benzoyl peroxide (BPO) in the presence of N-tert-butyl--isopropylnitrone as nitroxide precursor is well-controlled provided that a prereaction between the nitrone ... [more ▼]

The styrene polymerization initiated by benzoyl peroxide (BPO) in the presence of N-tert-butyl--isopropylnitrone as nitroxide precursor is well-controlled provided that a prereaction between the nitrone and BPO is carried out in suitable conditions prior to polymerization at a higher temperature. Electron spin resonance (ESR) spectroscopy was implemented to probe the nitroxides formed during both steps, that is, the prereaction and polymerization, and to get crucial information regarding the structure of the nitroxides responsible for the polymerization control. ESR studies combined with first principles calculations have evidenced that nitroxides observed during the prereaction in the presence of styrene and during the polymerization steps consist of a mixture of two macronitroxides. One is formed by the addition of a growing polystyrene chain to the nitrone as would be expected. However, the second one results from the addition of a polystyrene chain to tert-butyl nitroso that is in situ formed presumably by decomposition of the first macronitroxide type. [less ▲]

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See detailMagnetic hybrid materials for triggered drug delivery and optical properties of intraocular lens
Liu, Ji ULg; Jérôme, Christine ULg; Detrembleur, Christophe ULg et al

Conference (2013, March 20)

Mesoporous silica nanoparticles have great potential for drug delivery system (DDS) due to their large volume for encapsulation of guest molecules in the porous channels. Due to the specific magnetic ... [more ▼]

Mesoporous silica nanoparticles have great potential for drug delivery system (DDS) due to their large volume for encapsulation of guest molecules in the porous channels. Due to the specific magnetic responsiveness, magnetic nanoparticles can penetrate body tissues under a magnetic guidance, providing a potential platform for magnetic-directed DDS. Furthermore, a sharp local heating can be obtained for superparamagnetic nanoparticles when exposed to an alternating magnetic field (AMF). This specific property opens up the possibility of the application in tumor treatments. Here, we fabricated maghemite/SiO2 mesoporous nanohybrids DDS with phase-changed molecules as gate-keepers. The channels were envisaged to be closed in the biological systems during the delivery; however, opened when exposed to external heating or internal heating from hyperthermia generated by the maghemite cores. Thus the uploaded drug can diffuse into the surrounding medium. MTS assay showed a good cytocompatibility of the vehicles in both mouse L929 cells and cancer MEL-5 cells, and also internalization into MEL-5 cells was confirmed by Fluoresce microscopy, fluoresce-activated cell sorting (FACS) and TEM techniques. The release of drugs can be controlled by varying the concentration of the nanohybrids vehicles, the period of AMF treatment, or both. In-vivo triggered-release of doxorubicin into MEL-5 cells was confirmed by the sharp decrease in cell viability. This DDS can be designed for controlled release to an urgent physiological need via chemotherapy, hyperthermia therapy, or both. [less ▲]

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See detailThermally stable bulk heterojunction solar cells based on cross-linkable acrylate-functionalized polythiophene diblock copolymers
Ouhib, Farid ULg; Tomassetti, Mirco ULg; Manca, Jean et al

in Macromolecules (2013), 46(3), 785-795

We report on the synthesis of new thermally cross-linkable all-conjugated diblock copolymers composed of a poly(3-hexylthiophene) (P3HT) block and an acrylate-functionalized polythiophene block. These ... [more ▼]

We report on the synthesis of new thermally cross-linkable all-conjugated diblock copolymers composed of a poly(3-hexylthiophene) (P3HT) block and an acrylate-functionalized polythiophene block. These copolymers are then used in bulk heterojunction (BHJ) solar cells with [6,6]-phenyl C61-butyric acid methyl ester (PCBM), and their photovoltaic performances are compared with standard P3HT/PCBM devices. Thermal cross-linking of the functional copolymers/PCBM blends is performed to improve the thermal stability of the active layer. BHJ photovoltaic cells with cross-linkable copolymers and PCBM show initial power conversion efficiencies slightly lower than that of P3HT devices. However, solar cells with cross-linkable copolymers retain more than 85% of their initial power efficiency value after 165 h of thermal annealing (accelerated aging test), whereas the same devices with P3HT retain less than 65% of their initial power efficiency. This improvement of the thermal stability of BHJ photovoltaic cells is the result of the polymer network that hampers PCBM diffusion and phase separation, as confirmed with TEM and AFM analysis of the microscopic morphology. Such an improvement is mostly observed when using a cross-linkable P3HT with a short spacer between the acrylate group and the polythiophene backbone. [less ▲]

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See detailPhotochemical properties and activity of water-soluble polymer/C60 nanohybrids for photodynamic therapy
Hurtgen, Marie ULg; Debuigne, Antoine ULg; Hoebeke, Maryse ULg et al

in Macromolecular Bioscience (2013), 13(1), 106-115

Water-soluble star-like poly(vinyl alcohol)/C60 and poly{[poly(ethylene glycol) acrylate]-co- (vinyl acetate)}/C60 nanohybrids are prepared by grafting macroradicals onto C60 and are assessed as ... [more ▼]

Water-soluble star-like poly(vinyl alcohol)/C60 and poly{[poly(ethylene glycol) acrylate]-co- (vinyl acetate)}/C60 nanohybrids are prepared by grafting macroradicals onto C60 and are assessed as photosensitizers for photodynamic therapy. The photophysical and biological properties of both nanohybrids highlight key characteristics influencing their overall efficiency. The macromolecular structure (linear/graft) and nature (presence/absence of hydroxyl groups) of the polymeric arms respectively impact the photodynamic activity and the stealthiness of the nanohybrids. The advantages of both nanohybrids are encountered in a third one, poly[(Nvinylpyrrolidone)- co-(vinyl acetate)]/C60, which has linear grafts without hydroxyl groups, and shows a better photodynamic activity. [less ▲]

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See detailMultifunctional architectured materials for electromagnetic absorption
Bollen, P.; Quiévy, N.; Huynen, I. et al

in Scripta Materialia (2013), 68(1), 50-54

A sandwich structure involving a honeycomb core filled with a carbon nanotube-reinforced polymer foam and glass fiber-reinforced composite face sheets has been developed in order to combine high ... [more ▼]

A sandwich structure involving a honeycomb core filled with a carbon nanotube-reinforced polymer foam and glass fiber-reinforced composite face sheets has been developed in order to combine high electromagnetic absorption and high mechanical performance. The large electromagnetic absorption is attained by simultaneously minimizing the reflection and transmission, which, in terms of effective material properties, requires a low dielectric constant and a conductivity around 1 S m−1. The sandwich offers also high stiffness versus density performance. [less ▲]

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See detailCatechols as versatile platforms in polymer chemistry
Faure, Emilie; Falentin-Daudré, Céline; Jérôme, Christine ULg et al

in Progress in Polymer Science (2013), 38(1), 236-270

Catechols represent an important and versatile building block for the design of mussel-inspired synthetic adhesives and coatings. Indeed, their ability to establish large panoply of interactions with both ... [more ▼]

Catechols represent an important and versatile building block for the design of mussel-inspired synthetic adhesives and coatings. Indeed, their ability to establish large panoply of interactions with both organic and inorganic substrates has promoted catechol as a universal anchor for surface modifications. In addition to its pivotal role in adhesive interfaces, the catechol unit recently emerged as a powerful building block for the preparation of a large range of polymeric materials with intriguing structures and fascinating properties. The importance of catechols as efficient anchoring groups has been highlighted in recent excellent reviews partly dedicated to the characterization of their adhesive mechanisms onto surfaces and to their applications. The aim of this paper is to review for the first time the main synthetic approaches developed for the design of novel catechol-based polymer materials. We will also highlight the importance of these groups as versatile platforms for further functionalization of the macromolecular structures, but also surfaces. This will be illustrated by briefly discussing some advanced applications developed from these catechol-modified polymers. The review is organized according to the chemical structure of the functionalized catechol polymers. Chapter 1 discusses polymers bearing catechols embedded into the polymer main chain. Chapter 2 focuses on the attachment of catechol moieties as pendant groups and Chapter 3 describes the different approaches for incorporation of the catechol unit at the extremity of well-defined polymers. [less ▲]

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See detailSynthesis of poly(vinyl acetate)-b-poly(vinyl chloride) block copolymers by cobalt-mediated radical polymerization (CMRP)
Piette, Yasmine; Debuigne, Antoine ULg; Bodart, Vinent et al

in Polymer Chemistry (2013), 4(5), 1685-1693

The synthesis of poly(vinyl acetate)-b-poly(vinyl chloride) (PVAc-b-PVC) block copolymers by Cobalt-Mediated Radical Polymerization (CMRP) is investigated for the first time in this paper. A PVAc–Co(acac ... [more ▼]

The synthesis of poly(vinyl acetate)-b-poly(vinyl chloride) (PVAc-b-PVC) block copolymers by Cobalt-Mediated Radical Polymerization (CMRP) is investigated for the first time in this paper. A PVAc–Co(acac)2 macroinitiator is prepared by CMRP using the V-70/Co(acac)2 binary system or a preformed alkylcobalt(III) compound. Then, the block copolymerization occurs in the bulk at 40 °C by the addition of VC. The addition of water to the polymerization medium or the slow generation of alkyl radicals during the whole polymerization is beneficial to the process by consuming part of the excess of deactivator (Co(acac)2) that blocks the polymer chains into the dormant form. Dynamic light scattering (DLS) measurements and AFM analyses evidence that the PVAc-b-PVC forms core–shell micelles in a selective solvent of the PVAc block, i.e. methanol, evidencing the blocky structure of the copolymer. PVAc-b-P(VC-co-VAc) copolymers are also successfully prepared by initiating the radical copolymerization of VC and VAc at 40 °C from a PVAc–Co(acac)2 macroinitiator. [less ▲]

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See detailFunctional nanogels as platforms for imparting antibacterial, antibiofilm, and antiadhesion activities to stainless steel
Faure, Emilie ULg; Falentin, Céline ULg; Svaldo Lanero, Tiziana ULg et al

in Advanced Functional Materials (2012), 22(24), 5271-5282

In this work, long-term antibacterial, antiadhesion, and antibiofilm activities are afforded to industrial stainless steel surfaces following a green and bio-inspired strategy. Starting from catechol ... [more ▼]

In this work, long-term antibacterial, antiadhesion, and antibiofilm activities are afforded to industrial stainless steel surfaces following a green and bio-inspired strategy. Starting from catechol bearing synthetic polymers, the film cross-linking and the grafting of active (bio)molecules are possible under environmentally friendly conditions (in aqueous media and at room temperature). A bio-inspired polyelectrolyte, a polycation-bearing catechol, is used as the film-anchoring polymer while a poly(methacrylamide)-bearing quinone groups serves as the cross-linking agent in combination with a polymer bearing primary amine groups. The amine/quinone reaction is exploited to prepare stable solutions of nanogels in water at room temperature that can be easily deposited to stainless steel. This coating provides quinonefunctionalized surfaces that are then used to covalently anchor active (bio) molecules (antibiofi lm enzyme and antiadhesion polymer) through thiol/ quinone reactions. [less ▲]

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See detailCobalt-mediated radical (co)polymerization of vinyl chloride and vinyl acetate
Piette, Yasmine; Debuigne, Antoine ULg; Jérôme, Christine ULg et al

in Polymer Chemistry (2012), 3(10), 2880-2891

The cobalt mediated radical polymerization (CMRP) of vinyl chloride (VC) in the presence of bis(acetylacetonato)cobalt(II) (Co(acac)2) as a controlling agent is presented for the first time. Using an ... [more ▼]

The cobalt mediated radical polymerization (CMRP) of vinyl chloride (VC) in the presence of bis(acetylacetonato)cobalt(II) (Co(acac)2) as a controlling agent is presented for the first time. Using an alkyl-Co(III) compound (R0–(CH2–CHOAc)<4–Co(acac)2; R0 = (H3C)2(OCH3)C–CH2–C(CH3)(CN)–) as an initiator, the bulk polymerization under non-isotherm conditions is controlled. 1H NMR spectra of the resulting PVC show that the CMRP process does not significantly affect the level of defects compared to a PVC prepared by a conventional free radical polymerization at the same temperature. Using the same alkyl-cobalt(III) compound, the copolymerization of VC and VAc is controlled at 40 °C provided that enough VAc (about 40 mol%) is present in the polymerization medium to moderate the VC polymerization. In line with reactivity ratios, VC is preferentially incorporated in the polymer at the early stages of the polymerization, leading to copolymers with a high VC content at moderate conversions. This is the first report of a CMRP of VC and of the synthesis of well-defined statistical PVC-co-PVAc copolymers by this technique. [less ▲]

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