References of "Jérôme, Christine"
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See detailMacroporous poly(ionic liquid)/ionic liquid gels via CO2-based emulsion-templating polymerization
Mathieu, Kevin ULiege; Jérôme, Christine ULiege; Debuigne, Antoine ULiege

in Polymer Chemistry (in press)

Structuring poly(ionic liquid)s (PILs) into porous materials or swelling PILs with free ionic liquids (ILs) has received specific attention recently and contributed to improve the performances of these ... [more ▼]

Structuring poly(ionic liquid)s (PILs) into porous materials or swelling PILs with free ionic liquids (ILs) has received specific attention recently and contributed to improve the performances of these materials used in a wide range of applications. The present work aims to take benefit of both approaches and produce macroporous PIL/IL gels in a single step through an innovative emulsion-templated polymerization method based on supercritical carbon dioxide (scCO2). More precisely, ILs vinyl monomers and crosslinkers were polymerized in the presence of non polymerizable ILs within the outer phase of a CO2-in-ILs high internal phase emulsion (HIPE). Specific macromolecular surfactants were synthesized by controlled radical polymerization techniques and tested for the stabilization of the CO2-in-ILs emulsions. While optimizing the polymerization conditions, we found that adding a limited amount of water in the medium was beneficial for the emulsion stability. Overall, this straightforward process gave access to macroporous polyHIPEs composed of poly(vinyl imidazolium) networks swollen by ‘free’ vinyl imidazolium-based ILs having interesting properties such as switchable polarity upon simple anion exchange reaction. [less ▲]

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See detailTetrabutyl ammonium salts: cheap catalysts for the facile and selective synthesis of a-alkylidene cyclic carbonates from CO2 and alkynol
Méreau, Raphaël; Grignard, Bruno ULiege; Boyaval, Amélie ULiege et al

in ChemCatChem (in press)

n-tetrabutyl ammonium organic salts are used for the first time as catalysts for the coupling of CO2 with 2-methyl-3-butyn-2-ol to form α-methylene cyclic carbonate. The final yields could reach 98% in ... [more ▼]

n-tetrabutyl ammonium organic salts are used for the first time as catalysts for the coupling of CO2 with 2-methyl-3-butyn-2-ol to form α-methylene cyclic carbonate. The final yields could reach 98% in less than 10 hours at 353K and 3MPa under solvent free conditions. A particular synergistic effect between the cation and the anion of the organocatalyst is demonstrated through catalyst screening. Online kinetic studies by ATR-IR spectroscopy correlated to DFT calculations reveal a compelling evolution of the solvation of the catalyst during the reaction that provide an understanding of the underlying reason for the observed unique kinetics and selectivity. Such in-depth fundamental mechanistic and kinetic studies enable determining and comprehending the key parameters favouring the design of novel highly active and selective catalysts for the valorisation [less ▲]

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See detailUnique alternating peptide-peptoid copolymers from dipeptides via Ugi reaction in water
Al Samad, Assala ULiege; De Winter, Julien; Gergaux, Pascal et al

in Chemical Communications (2017), 53(90), 12240-12243

Herein, we developed a strainghtforward aqueous synthesis of unprecedented alternating peptide-peptoid copolymers via Ugi four-component reaction applied to dipeptides. Functional peptide-peptoid ... [more ▼]

Herein, we developed a strainghtforward aqueous synthesis of unprecedented alternating peptide-peptoid copolymers via Ugi four-component reaction applied to dipeptides. Functional peptide-peptoid copolymers as well as block copolymers were produced in a single step in the presence of acrylic acid and carboxylic acid-terminated poly(ethylene glycol). The thermoresponsiveness of these polymers is highlighted [less ▲]

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See detailDevelopment and evaluation of injectable nanosized drug delivery systems for apigenin
Karim, Reatul ULiege; Palazzo, Claudio ULiege; Laloy, Julie et al

in International Journal of Pharmaceutics (2017), 532(2), 757-768

The purpose of this study was to develop different injectable nanosized drug delivery systems (NDDSs) i.e. liposome, lipid nanocapsule (LNC) and polymeric nanocapsule (PNC) encapsulating apigenin (AG) and ... [more ▼]

The purpose of this study was to develop different injectable nanosized drug delivery systems (NDDSs) i.e. liposome, lipid nanocapsule (LNC) and polymeric nanocapsule (PNC) encapsulating apigenin (AG) and compare their characteristics to identify the nanovector(s) that can deliver the largest quantity of AG while being biocompatible. Two liposomes with different surface characteristics (cationic and anionic), a LNC and a PNC were prepared. A novel tocopherol modified poly(ethylene glycol)-b-polyphosphate block-copolymer was used for the first time for the PNC preparation. The NDDSs were compared by their physicochemical characteristics, AG release, storage stability, stability in serum, complement consumption and toxicity against a human macrovascular endothelial cell line (EAhy926). The diameter and surface charge of the NDDSs were comparable with previously reported injectable nanocarriers. The NDDSs showed good encapsulation efficiency and drug loading. Moreover, the NDDSs were stable during storage and in fetal bovine serum for extended periods, showed low complement consumption and were non-toxic to EAhy926 cells up to high concentrations. Therefore, they can be considered as potential injectable nanocarriers of AG. Due to less pronounced burst effect and extended release characteristics, the nanocapsules could be favorable approaches for achieving prolonged pharmacological activity of AG using injectable NDDS. [less ▲]

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See detailBioinspired redox-active catechol-bearing polymers as ultra-robust organic cathodes for lithium storage
Patil, Nagaraj ULiege; Aqil, Abdelhafid ULiege; Ouhib, Farid ULiege et al

in Advanced Materials (2017), 29(40), 1703373

Redox-active catechols are bioinspired precursors for ortho-quinones that are characterized by higher discharge potentials than para-quinones, the latter being extensively used as organic cathode ... [more ▼]

Redox-active catechols are bioinspired precursors for ortho-quinones that are characterized by higher discharge potentials than para-quinones, the latter being extensively used as organic cathode materials for lithium ion batteries (LIBs). Here, this study demonstrates that the rational molecular design of copolymers bearing catechol- and Li+ ion-conducting anionic pendants endow redox-active polymers (RAPs) with ultrarobust electrochemical energy storage features when combined to carbon nanotubes as a flexible, binder-, and metal current collector-free buckypaper electrode. The importance of the structure and functionality of the RAPs on the battery performances in LIBs is discussed. The structure-optimized RAPs can store high-capacities of 360 mA h g−1 at 5C and 320 mA h g−1 at 30C in LIBs. The high ion and electron mobilities within the buckypaper also enable to register 96 mA h g−1 (24% capacity retention) at an extreme C-rate of 600C (6 s for total discharge). Moreover, excellent cyclability is noted with a capacity retention of 98% over 3400 cycles at 30C. The high capacity, superior active-material utilization, ultralong cyclability, and excellent rate performances of RAPs-based electrode clearly rival most of the state-of-the-art Li+ ion organic cathodes, and opens up new horizons for large-scalable fabrication of electrode materials for ultrarobust Li storage. [less ▲]

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See detailReinforced poly(hydroxyurethane) thermosets as high performance adhesives for aluminum substrates
Panchireddy, Satyannarayana ULiege; Thomassin, Jean-Michel ULiege; Grignard, Bruno ULiege et al

in Polymer Chemistry (2017), 8(38), 5897-5909

Poly(hydroxyurethane) (PHU) thermosets reinforced with (functional) nanofillers were developed to design high performance adhesives for bare aluminum. Solvent-free cyclic carbonate/amine/PDMS formulations ... [more ▼]

Poly(hydroxyurethane) (PHU) thermosets reinforced with (functional) nanofillers were developed to design high performance adhesives for bare aluminum. Solvent-free cyclic carbonate/amine/PDMS formulations loaded with native, epoxy- or cyclic carbonate-functionalized ZnO nanofillers were premixed before deposition and thermal curing onto Al. The results highlight that the addition of PDMS prevents PHUs from delamination of the Al surface by increasing the adhesive hydrophobicity and thus limiting the water uptake. The dispersion of functional fillers within PHUs improves their thermal and mechanical properties. Benchmarking of the adhesive performances of the reinforced PHU glues with existing PHU formulations attests for the benefits of dispersing functional fillers and PDMS within the resin and evidences a 270% increase of the shear strength of reinforced PHUs adhesives compared to formulations reported in the literature. [less ▲]

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See detailOn the phase behaviour of oxetane-CO2 and propargylic alcohols-CO2 binary mixtures by in situ infrared micro-spectrometry
Zaky, Mohamed; Boyaval, Amélie ULiege; Grignard, Bruno ULiege et al

in Journal of Supercritical Fluids (2017), 128

The phase behaviour of carbon dioxide/propargylic alcohols and carbon dioxide/oxetanes mixtures has been investigated using in-situ FTIR microspectrometry that allows us determining the evolution of the ... [more ▼]

The phase behaviour of carbon dioxide/propargylic alcohols and carbon dioxide/oxetanes mixtures has been investigated using in-situ FTIR microspectrometry that allows us determining the evolution of the concentration of each component in the liquid phase as a function of temperature and pressure. It was at the same time possible to look inside the cell and to visualize the expansion of the liquid phase during the increase of the pressure. The measurements were performed at three different temperatures (40, 70 and 100◦C) for pressures ranging between 0.1 and 15 MPa. Propargylic alcohol (PA), 2-methyl-3-butyn-2-ol (MBOL), 3-butyn-1-ol (BOL) and trimethylene oxide (TMO) were selected as these molecules are used in the synthesis of cyclic or polycarbonates by coupling with CO2. Thus, we determined the CO2 sorption and the concentration of the substrate in the liquid phase. Thanks to these measurements, we established the pressure-composition phase diagram for the liquid phase of these substrate/CO2 binary mixtures. [less ▲]

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See detailMerging supercritical carbon dioxide and organocatalysis for the precision and green synthesis of poly(lactide)-based (co)polymers
Grignard, Bruno ULiege; De Winter, Julien; Gerbaux, Pascal et al

in European Polymer Journal (2017), 95

Well-defined poly(lactide)-based block copolymers were synthesized by a heterogeneous solvent and metal-free green approach by using organocatalysts in supercritical carbon dioxide (scCO2). We first ... [more ▼]

Well-defined poly(lactide)-based block copolymers were synthesized by a heterogeneous solvent and metal-free green approach by using organocatalysts in supercritical carbon dioxide (scCO2). We first report on the homopolymerization of both L- and D,L- lactide by organocatalyzed Ring-Opening Polymerization (o-ROP) by using a bicomponent organocatalyst composed of a thiourea derivative and various tertiary amines as cocatalysts. Control over the molar mass and dispersity is achieved until high monomer conversion although the polylactides are insoluble in the polymerization medium. The precision synthesis of PLA-based block copolymers from various CO2-phobic hydroxyl end-capped macroinitiators such as polyethylene glycol, polycaprolactone, polybutylene succinate and polyphosphoester was then reported. Merging scCO2 with this organocatalytic system provides therefore a unique tool for the design under solvent-free conditions of poly(lactide)-based block copolymers that are insoluble in scCO2. [less ▲]

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See detailGoing Inside Structural and Physicochemical Properties of Polymers using Ion Mobility-Mass Spectrometry
Haler, Jean ULiege; de la Rosa, Victor R.; Far, Johann ULiege et al

Conference (2017, September 06)

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See detailVINYLIC COPOLYMERS FOR PH-SENSITIVE LIPID NANOCAPSULES
Pautu, Vincent ULiege; Lepeltier, Elise; Debuigne, Antoine ULiege et al

Poster (2017, September)

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See detailWell-defined polyvinylamine-based copolymers: synthesis by organometallic-mediated radical polymerization and use in gene transfection
Debuigne, Antoine ULiege; Dréan, Mathilde; Detrembleur, Christophe ULiege et al

Conference (2017, August 22)

Polyvinylamine (PVAm) presents valuable properties like affinity for many supports, pH responsiveness, metal binding capacity, polyelectrolytes complexation, and is used in various applications including ... [more ▼]

Polyvinylamine (PVAm) presents valuable properties like affinity for many supports, pH responsiveness, metal binding capacity, polyelectrolytes complexation, and is used in various applications including coatings, water purification or gas membrane separation. PVAm is commonly prepared by free radical polymerization of N-vinyl monomers followed by deprotection and release of the masked amino functions. However, examples of controlled synthesis of polyvinylamine-based copolymers are scarce because of the high reactivity of the propagating radicals deriving from non-conjugated N-vinyl monomers due to the lack of resonance stabilization. The present communication aims at reporting an efficient platform for producing tailor-made PVAms via organometallic-mediated radical polymerization (OMRP) of N-vinylacetamides followed by hydrolysis of the pendent amide moieties. In this case, cobalt(II) acetylacetonate was successfully used as controlling agent. The synthesis of a series of well-defined homopolymers, statistical and block copolymers with pendent primary and/or secondary amines having low dispersities, predictable molar masses and precise compositions, will be described. Finally, we will discuss the possible use of these polyvinylamine-containing copolymers as gene transfection agents. Some of them demonstrated high DNA transfection level in combination with high cell viability. [less ▲]

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See detailCO2-sourced α-alkylidene cyclic carbonates: a Step forward in the quest for functional regioregular poly(urethane)s and poly(carbonate)s
Gennen, Sandro ULiege; Grignard, Bruno ULiege; Tassaing, Thierry et al

in Angewandte Chemie International Edition (2017), 56(35), 1039410398

We describe a robust platform for the synthesis of a large diversity of novel functional CO2 -sourced polymers by exploiting the regio-controlled and site selective ring-opening of α- alkylidene ... [more ▼]

We describe a robust platform for the synthesis of a large diversity of novel functional CO2 -sourced polymers by exploiting the regio-controlled and site selective ring-opening of α- alkylidene carbonates by various nucleophiles. The remarkable reactivity of α-alkylidene carbonates is dictated by the exocyclic olefinic group that selectively orients the cyclic carbonate ring- opening with the formation of an enol species. The polyaddition of CO2 -sourced bis-α-alkylidene carbonates (bis-αCCs) with primary and secondary diamines provides novel regioregular functional poly(urethane)s. The reactivity of bis-αCCs is also exploited for producing new poly(β-oxo-carbonate)s by organocatalyzed polyaddition with a diol. All polyadditions were feasible under ambient conditions. This synthesis platform provides new functional variants of world-class leading polymers families (polyurethanes, polycarbonates) and valorises CO2 as a chemical feedstock. [less ▲]

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See detailMild synthesis of poly(HEMA)-networks as well-defined nanoparticles in supercritical carbon dioxide
Parilti, Rahmet ULiege; Alaimo, David; Grignard, Bruno ULiege et al

in Journal of Materials Chemistry B (2017), 5(29), 5806-5815

Free-radical dispersion polymerisation of 2-hydroxyethyl methacrylate was carried out in supercritical carbon dioxide (scCO2) in the presence of stabilisers based on polyethylene oxide (PEO) and poly ... [more ▼]

Free-radical dispersion polymerisation of 2-hydroxyethyl methacrylate was carried out in supercritical carbon dioxide (scCO2) in the presence of stabilisers based on polyethylene oxide (PEO) and poly(heptadecafluorodecyl acrylate) (PFDA). Different architectures of copolymers (random, palm-tree and diblock) were tested for their surface tension, cloud point and as a stabilising agent. The diblock architecture was found to be the best candidate resulting in poly(HEMA) spherical particles with a size of 316 nm. Furthermore, the effect of the CO2-phobic block (PEO) in the diblock architecture was investigated by using three different chain lengths (1000, 2000, 5000 g mol−1). By optimizing the stabiliser composition and structure, mild reaction conditions have been identified allowing us to obtain well-defined spherical cross-linked poly(HEMA) particles with a mean diameter of unprecedented low size (216 nm) at a temperature as low as 35 °C. [less ▲]

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See detailInnovative polyelectrolytes/poly(ionic liquid)s for energy and environment
Ajjan, Fátima N.; Ambrogi, Martina; Tiruye, Girum Ayalneh et al

in Polymer International (2017), 66(8), 1119-1126

This manuscript presents the work carried out within the European Project RENAISSANCE-ITN, which was dedicated to the development of innovative polyelectrolytes for energy and environmental applications ... [more ▼]

This manuscript presents the work carried out within the European Project RENAISSANCE-ITN, which was dedicated to the development of innovative polyelectrolytes for energy and environmental applications. Within the project different types of innovative polyelectrolytes were synthesized such as poly(ionic liquid)s coming from renewable or natural ions, thiazolium cations, cathechol functionalities or from a new generation of cheap deep-eutectic monomers. Further, macromolecular architectures such as new poly(ionic liquid) block copolymers and new (semi)conducting polymer/polyelectrolyte complexes were also developed. As the final goal, the application of these innovative polymers in energy and environment was investigated. Important advances in energy storage technologies included the development of new carbonaceous materials, new lignin/conducting polymer biopolymer electrodes, new iongels and single-ion conducting polymer electrolytes for supercapacitors and batteries and new poly(ionic liquid) binders for batteries. On the other hand, the use of the innovative polyelectrolytes into sustainable environmental technologies led to the development of new liquid and dry water, new materials for water cleaning technologies such as floculants, oil absorbers, new recyclable organocatalysts platform and multifunctional polymer coatings with antifouling and antimicrobial properties. All in all this article demonstrates the potential of the poly(ionic liquid)s for high-value applications in Energy & Enviromental areas. [less ▲]

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See detailBio- and CO2-sourced polyhydroxyurethanes for hydrogels coatings, foams and high performance adhesives
Gennen, Sandro ULiege; Panchireddy, Satyannarayana ULiege; Grignard, Bruno ULiege et al

Poster (2017, June 09)

Due to concerns about global warming combined with the decrease of fossil resources, the chemical transformation of carbon dioxide (CO2) 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 (CO2) into added-value products has gained interest in both academic and industrial fields. Indeed, CO2 can be viewed as a cheap, non-toxic and renewable C1 building block precursor of sophisticated organic molecules and polymers. One representative example of CO2 transformation includes the synthesis of various (bis)cyclic carbonates via CO2/epoxide coupling.1-3 Bis-cyclic carbonates were then valorized as monomers for the synthesis of series of novel low carbon footprint poly(hydroxyurethane)s (PHUs). These polymers are now exploited to produce sustainable materials including foams for thermal insulation,4 hydrogels (for potential biomedical use)5 and high performance adhesives and glues (for metal, glass and wood). [less ▲]

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See detailPolyphosphoesters: new trends in synthesis and drug delivery applications
Jérôme, Christine ULiege

Conference (2017, May 24)

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See detailMultifunctional poly(ionic liquid)s: from synthesis to applications in energy and environment
Detrembleur, Christophe ULiege; Patil, Nagaraj ULiege; Debuigne, Antoine ULiege et al

Conference (2017, May 24)

Poly(ionic liquid)s (PILs) are a subclass of polyelectrolytes that gained an enabling role in many fields of polymer chemistry and material science. PILs combine the unique properties of ionic liquids ... [more ▼]

Poly(ionic liquid)s (PILs) are a subclass of polyelectrolytes that gained an enabling role in many fields of polymer chemistry and material science. PILs combine the unique properties of ionic liquids with the flexibility and properties of macromolecules, and provide novel attractive functions. Recently, the precision design of novel PILs by controlled/living polymerization (CLP) techniques was intensively searched for developing emerging applications. This talk will first discuss recent routes for the precision synthesis of all vinyl-imidazolium based (co)polymers in water or in organic media under non-demanding experimental conditions. We will then describe the preparation of innovative redox and surface active PILs, and show the potential of these PILs in battery applications and for multifunctional coatings. More specifically, we will show how macromolecular engineering can be exploited for designing innovative polymer cathodes for ultra-high performance Li storage with unprecedented performances (high capacities and ultra-long life-span over more than 3000 cycles at an extreme current-rate). This innovative and effective molecular design for polymer cathodes opens up new horizons in developing an economical and environmentally benign platform for large-scalable fabrication of high performance batteries. [less ▲]

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See detailDesign of polyphosphoester-based drug delivery systems by efficient thiol-ene reaction
Riva, Raphaël ULiege; Vanslambrouck, Stéphanie; Ergül, Zeynep ULiege et al

Poster (2017, May 23)

Thanks to their biocompatibility, biodegradability and their structure similar to natural biomacromolecules, polyphosphoesters (PPE) are appealing polymers for biomedical applications. In contrast to ... [more ▼]

Thanks to their biocompatibility, biodegradability and their structure similar to natural biomacromolecules, polyphosphoesters (PPE) are appealing polymers for biomedical applications. In contrast to polyesters, PPE properties and functionality are easily tuned via the chemical nature of the lateral chains. To enhance the drug loading capacity of PPE-based micelles used as carriers for the delivery of poorly soluble drugs, an efficient strategy to increase the lipophilicity of the PPE block of polyethylene oxide (PEO)-b-PPE amphiphilic copolymers has been investigated. A PEO-b-PPE copolymer bearing pendant vinyl groups along the PPE block was synthesized and then modified by thiol-ene click reaction with thiols bearing either a long linear alkyl chain (dodecyl) or a tocopherol moiety. Ketoconazole was used as model for hydrophobic drugs. Comparison of the loading contents and release profiles with PEO-b-PPE bearing shorter pendant groups is presented evidencing the key role of the structure of the pendant group on the PPE backbone. Finally, the low cytotoxicity of these novel PEO-b-PPE copolymers was also demonstrated. The tocopherol derivative was evidenced as particularly promising for drug delivery systems. [less ▲]

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