References of "Detrembleur, Christophe"
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See detailRAFT polymerization of an alkoxyamine bearing acrylate, towards a well-defined redox active polyacrylate
Aqil, Mohamed ULg; Aqil, Abdelhafid ULg; Ouhib, Farid ULg et al

in RSC Advances (2015), 5(103), 85035-85038

A new strategy for the synthesis of a well-defined redox active poly- mer, a polyacrylate bearing TEMPO, and its grafting onto a gold substrate is described. It consists of polymerizing an acrylate ... [more ▼]

A new strategy for the synthesis of a well-defined redox active poly- mer, a polyacrylate bearing TEMPO, and its grafting onto a gold substrate is described. It consists of polymerizing an acrylate bearing an alkoxyamine by RAFT, followed by aminolysis of the trithiocar- bonate chain-end into a thiol that is exploited for the polymer grafting onto the gold sensor. Thermal activation of the alkoxyamine under air provides the redox polymer with a high yield. Its electroactivity is evaluated by a electrochemical quartz crystal microbalance (EQCM). [less ▲]

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See detailConducting, self-assembled, nacre-mimetic polymer/clay nanocomposites
Mäkiniemi, Roi Oskari; Das, Paramita; Hönders, Daniel et al

in ACS Applied Materials and Interfaces (2015), 7(29), 15681-15685

We demonstrate electrically and ionically conducting nacre-mimetic nanocomposites prepared using self-assembly of synthetic nanoclay in combination with PEDOT:PSS and a poly(ionic liquid) polymer from ... [more ▼]

We demonstrate electrically and ionically conducting nacre-mimetic nanocomposites prepared using self-assembly of synthetic nanoclay in combination with PEDOT:PSS and a poly(ionic liquid) polymer from aqueous dispersions. The resulting nacre-mimetics show high degrees of mesoscale order and combine high stiffness and high strength. In terms of conductivities, the resulting hybrids exceed simple additive behavior and display synergetic conductivities due to high levels of interfaces and anisotropic conductivity pathways. The approach highlights the integration of relevant functionalities into stiff and strong bioinspired materials, and shows that synergetic properties beyond mechanical performance can be realized in advanced multifunctional nanocomposites using nacre-inspired design principles. [less ▲]

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See detailOrganocatalytic synthesis of bio-based cyclic carbonates from CO2 and vegetable oils
Alves, Margot ULg; Grignard, Bruno ULg; Gennen, Sandro ULg et al

in RSC Advances (2015), 5

Bio-based cyclic carbonates were synthesized by coupling CO2 with epoxidized linseed oil using a catalytic platform composed of a bicomponent organocatalyst. A screening of the catalytic activity of a ... [more ▼]

Bio-based cyclic carbonates were synthesized by coupling CO2 with epoxidized linseed oil using a catalytic platform composed of a bicomponent organocatalyst. A screening of the catalytic activity of a series of organic salts and ionic liquids used in combination with (multi)phenolic or fluorinated hydrogen bond donors was realized before highlighting the synergistic effect between the organocatalyst and the most efficient cocatalysts. These kinetics studies, followed by IR spectroscopy under pressure, enabled to optimize the reaction conditions and to provide quantitative formation of the cyclocarbonated vegetable oil in short reaction time without using any organic solvent. [less ▲]

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See detailNanocomposite foams of polypropylene and carbon nanotubes: preparation, characterization, and evaluation of their performance as EMI absorbers
Tran, Minh-Phuong; Thomassin, Jean-Michel ULg; Alexandre, Michaël et al

in Macromolecular Chemistry and Physics (2015), 216(12), 1302-1312

Highly expanded nanocomposite foams of polypropylene and carbon nanotubes (PP/CNT) are formed using supercritical carbon dioxide (scCO 2 ) technology. The foaming parameters (temperature, pressure) are ... [more ▼]

Highly expanded nanocomposite foams of polypropylene and carbon nanotubes (PP/CNT) are formed using supercritical carbon dioxide (scCO 2 ) technology. The foaming parameters (temperature, pressure) are investigated to establish their infl uence on the morphology of the resulting foams and their impact on the electrical con- ductivity. As promising electromagnetic-interference (EMI) absorbers, the EMI shielding performance of the foams is determined, and a preliminary relationship is established between foam morphology and the EMI shielding perfor- mance. The best candidates are highly expanded foams with a volume expansion of >25, containing 0.1 vol% CNTs; they are able to absorb more than 90% of the incident radiation between 25 and 40 GHz. [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 detailGraphene functionalization using electrografting for energy storage application
Aqil, Abdelhafid ULg; Ouhib, Farid ULg; Aqil, Mohamed ULg et al

Conference (2014, November 04)

Many methods have been developed in the last few decades to obtain high-quality graphene thin sheets. They are based on very different physicochemical processes. Here we demonstrate a novel one step and ... [more ▼]

Many methods have been developed in the last few decades to obtain high-quality graphene thin sheets. They are based on very different physicochemical processes. Here we demonstrate a novel one step and simple electrografting acrylate monomer method to exfoliate highly oriented pyrolytic graphite (HOPG) into thin nanoplatelets and even down to the single graphene sheet level. Among the high research activity in the area of surface modification, electrografting is a very powerful method which has received comparatively little attention. This is surprising because this technique has many attractive features for modification of conducting or semi-conducting surfaces. The main interest of the electrografting process is to solve the recurrent problem of the organic/substrates interface weakness. The electrografting warranties a robust polymer/substrates interface and offers the possibility to tailor the functionality of the grafted polymer film opening the door to a wide range of demanding technological applications. The graphene sheets obtained through electrografting process give a stable suspension in dimethyl formamide (DMF), and they can self-precipitate on the surface of substrates after adding water as an antisolvent due to their strong surface hydrophobicity. Interestingly, the continuous films obtained exhibit ultratransparency (∼98% transmittance), and the lateral size of the exfoliated graphene sheets observed by AFM ~1nm. Raman and TEM characterizations corroborate that the graphene sheets exfoliated by our electrochemical method preserve the intrinsic structure of grapheme and give preferentially monolayered graphene sheets. The electrochemical behaviour of the acrylate monomer grafted graphene sheets was evaluated in lithium-half cells with no addition of conductive additive or binder. The PAN grafted graphene dispersed in DMF was coated on Cu foil and dried in a vacuum oven at 55°C for 12h. After 200 cycles, the reversible capacity was still kept at 300mAh/g at the current density of 50mA/g. These results indicate that the prepared high quality graphene sheets possess good electrochemical performances for lithium storage. This work provides an efficient approach to obtain high-quality, cost-effective, and scalable production of “graphene ink”, which may pave a way toward future applications in lithium-ion batteries. [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 detailPrecision design of novel poly(ionic liquid) (co)polymers by cobalt-mediated radical polymerization (CMRP)
Cordella, Daniela ULg; Kermagoret, Anthony ULg; Debuigne, Antoine ULg et al

Poster (2014, May 20)

In recent years, poly(ionic liquid)s (PIL)s were found to take an enabling role in important fields of polymer chemistry and material science. PILs combine the unique properties of ionic liquids with the ... [more ▼]

In recent years, poly(ionic liquid)s (PIL)s were found to take an enabling role in important fields of polymer chemistry and material science. PILs combine the unique properties of ionic liquids with the flexibility and properties of macromolecular architectures giving rise to a new family of functional polymers that opens new area of applications such as polymer electrolytes in electrochemical devices, powerful dispersants and stabilizers, absorbing membranes, precursors for carbon materials, porous polymers, etc. In this communication, we will report on the implementation of organometallic-mediated radical polymerization (OMRP) technique for the precision synthesis of unprecedented PILS (co)polymers. We will discuss how an organocobalt complex can nicely control the growth of vinyl imidazolium chains and lead to PILS with predicted molar masses and low polydispersitiesunder mild experimental conditions. The huge potential of this system will be highlighted by describing the first one-pot synthesis of vinyl imidazolium-based block copolymers in heterogeneous conditions. This OMRP is unique for providing well-defined vinyl imidazolium based-copolymers that are not easily accessible by other controlled radical polymerization techniques, and opens therefore new rooms for advanced PILS applications. [less ▲]

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See detailSurface-immobilised anti-fouling block-copolymers: synthesis and characterization
Patil, Nagaraj ULg; Detrembleur, Christophe ULg; Jérôme, Christine ULg

Poster (2014, May 20)

Poly(ethylene glycol) (PEG)-based polymers have been widely employed in anti-fouling coating applications due to their robust bio-relevant properties including water solubility and biocompatibility ... [more ▼]

Poly(ethylene glycol) (PEG)-based polymers have been widely employed in anti-fouling coating applications due to their robust bio-relevant properties including water solubility and biocompatibility. However, limited by its poor adhesion towards surfaces, demands an addition modification strategies. Mussel adhesive proteins (MAPs) are potential models for adhesive polymers, which exhibits underwater adhesion towards dissimilar materials under environmentally challenging conditions. Most often experimentally simple, but structurally complex poly(dopamine) has been used as an analogues of MAPs for metal chelation, cross-linking and surface binding purposes. Inspired by MAPs, we have developed catechol-bearing copolymers for surface adhesion of stainless steel. This study aims at developing novel catechol-bearing, PEG-based block-copolymers by reversible addition-fragmentation chain transfer (RAFT) polymerization technique. PEGA used as macro-RAFT to prepare acetonide-protected catechol as second block. Deprotection of acetonide groups under acidic conditions produced functional block-copolymer with free catechols as pendant moieties. The self-assembling nature of amphiphilic block-copolymers was studied by 1H-NMR, DLS and TEM. Surface functionalization and anti-fouling experiments were performed in real time using quartz crystal microbalance coupled with dissipation (QCM-D). The copolymer upon oxidation yields reactive quinones, which can be exploited to cross-link with chitosan (also, polymers with free –NH2 and –SH groups), thereby producing nano(macro)gels. Benefited from inherent anti-microbial and anti-oxidative properties of chitosan and catechol-respectively, could result in potential materials for water purification systems, food packaging and medical devices. [less ▲]

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