References of "Jérôme, Christine"
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See detailDFT investigation of the reaction mechanism for the guanidine catalyzed ring-opening of cyclic carbonates by aromatic and alkyl-amines
Alves, Margot ULg; Méreau, Raphaël; Grignard, Bruno ULg et al

in RSC Advances (in press)

The guanidine catalysed aminolysis of propylene carbonate has been investigated using the density functional theory (DFT) and highlights that different reaction pathways are involved depending on the ... [more ▼]

The guanidine catalysed aminolysis of propylene carbonate has been investigated using the density functional theory (DFT) and highlights that different reaction pathways are involved depending on the aromatic or aliphatic nature of the amine. The structural ability of 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) to simultaneously give and receive protons was demonstrated by a detailed mechanistic investigation. The bifunctional activity (base/H-bond donor) of TBD significantly reduces the Gibbs energy of the reaction and allows understanding its higher efficiency compared to its methyl counterpart (MTBD). [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 (in press)

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 detailOrganometallic-mediated radical polymerization of 'less activated monomers': fundamentals, challenges and opportunities
Debuigne, Antoine ULg; Jérôme, Christine ULg; Detrembleur, Christophe ULg

in Polymer (in press)

Access to well-defined polymers made of the so-called ‘Less Activated Monomers’ (LAMs) via controlled radical polymerization has long been a challenge due to the lack of radical stabilizing group on the ... [more ▼]

Access to well-defined polymers made of the so-called ‘Less Activated Monomers’ (LAMs) via controlled radical polymerization has long been a challenge due to the lack of radical stabilizing group on the double bond of these monomers. This Feature Article summarizes substantial progress in the organometallic-mediated radical polymerization (OMRP) of this important class of monomers including vinyl esters, olefins, vinyl chloride, vinyl amides, or ionic-liquid vinyl monomers. It aims to provide a clear and comprehensive account of the fundamentals and challenges in the OMRP of LAMs as well as an overview of the resulting macromolecular engineering opportunities. The input of photochemistry, environmentally friendly solvents or flow reactors in OMRP is also presented. Finally, it emphasizes how some well-defined LAMs-based materials contributed to the development of specific applications notably in the fields of biomedicine or energy. [less ▲]

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See detailOrganocatalytic coupling of CO2 with a propargylic alcohol: a comprehensive study of the reaction mechanism combining in- situ ATR-IR spectroscopy and DFT calculations
Boyaval, Amélie ULg; Méreau, Raphaël; Grignard, Bruno ULg et al

in ChemSusChem (in press)

The metal-free coupling of propargylic alcohols with carbon dioxide catalysed by guanidine derivatives was investigated in detail through the combination of online kinetic studies by in-situ ATR-IR ... [more ▼]

The metal-free coupling of propargylic alcohols with carbon dioxide catalysed by guanidine derivatives was investigated in detail through the combination of online kinetic studies by in-situ ATR-IR spectroscopy and DFT calculations. Bicyclic guanidines, namely TBD and MTBD, are effective catalysts for the conversion of 2-methyl-3-butyn-2-ol to α-methylene cyclic carbonate and oxoalkyl acyclic carbonate under mild reaction conditions. The lower selectivity of TBD in comparison with MTBD towards the formation of α-methylene cyclic carbonate was elucidated from DFT calculations and is related to the bifunctional activity (base/H-bond donor) of TBD decreasing the Gibbs free energy of the reaction path for the formation of the acyclic carbonate. Introduction [less ▲]

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See detailOrganocatalytic coupling of CO2 with oxetane
Alves, Margot ULg; Grignard, Bruno ULg; Boyaval, Amélie ULg et al

in ChemSusChem (in press)

The organocatalytic coupling of CO2 with oxetanes is investigated under solvent-free conditions. The influence of the main reaction parameters (type of organocatalytic system, pressure and temperature) on ... [more ▼]

The organocatalytic coupling of CO2 with oxetanes is investigated under solvent-free conditions. The influence of the main reaction parameters (type of organocatalytic system, pressure and temperature) on the yield, the product formed and the selectivity of the reaction are discussed. An onium salt combined with a fluorinated alcohol promotes the efficient and selective organocatalytic synthesis of ?,?-hydroxyl oligocarbonates by coupling CO2 with oxetanes at 130°C and at a CO2 pressure as low as 2 MPa. NMR characterizations were correlated with MALDI-ToF analyses for elucidating the structure of the oligomers. Online FTIR studies under pressure, NMR titrations and DFT calculations allowed an in-depth understanding of the reaction mechanism. Finally, CO2- based poly(carbonate-co-urethane)s were synthesized by step- growth polymerization of hydroxyl telechelic oligocarbonates with MDI. The organocatalytic system described in this paper constitutes an innovative sustainable route to the selective preparation of hydroxyl telechelic carbonates, of high interest for many applications, notably for the polyurethane business, especially for coatings or foams. [less ▲]

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See detailSimultaneous synthesis and chemical functionalization of emulsion-templated porous polymers using nitroxide-terminated macromolecular surfactants
Mathieu, Kevin ULg; De Winter, Julien; Jérôme, Christine ULg et al

in Polymer Chemistry (2017), 8(11), 1850-1861

The design of functional 3D macroporous monoliths has become a necessity for a wide range of applications. Traditional post-modification strategies of porous materials are efficient but often consist in ... [more ▼]

The design of functional 3D macroporous monoliths has become a necessity for a wide range of applications. Traditional post-modification strategies of porous materials are efficient but often consist in tedious multi-steps processes. This work describes a straightforward macromolecular surfactant-assisted method for producing chemically functionalized macroporous polyHIPEs with interconnected structures. Accordingly, high internal phase emulsion-templated polymerizations were implemented in the presence of SG1-terminated amphiphilic copolymers prepared by nitroxide- mediated radical polymerization (NMP). The latter served as both stabilizers and functionalizing agents upon thermal activation of its terminal alkoxyamine and covalent anchoring of the released radical copolymer onto the walls of the scaffold. The effect of the polymerization temperature on the functionalization and openness of the final porous materials was explored. As a result, a range of open-cell styrene and acrylate-based polyHIPEs chemically grafted with PEO were obtained. Moreover, polyHIPEs were also decorated with alkyne-bearing PEO and subsequently modified via CuAAc click chemistry in order to demonstrate the potential of this macromolecular surfactants-assisted functionalization method. [less ▲]

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See detailEnolates in macromolecular science: current situation and future outlook
Lecomte, Philippe ULg; Jérôme, Christine ULg

in Zabicky, Jacob (Ed.) The Chemistry of Metal Enolates (Volume 2) (2017)

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See detailBioreducible cross-linked core polymer micelles enhance in vitro activity of methotrexate in breast cancer cells
Gulfam, Muhammad ULg; Matini, Teresa; Monteiro, Patrícia F et al

in Biomaterials Science (2017), 5(3), 532-550

Polymer micelles have emerged as promising carriers for controlled release applications, however, several limitations of micelle-based drug delivery have also been reported. To address these issues, we ... [more ▼]

Polymer micelles have emerged as promising carriers for controlled release applications, however, several limitations of micelle-based drug delivery have also been reported. To address these issues, we have synthesized a functional biodegradable and cytocompatible block copolymer based on methoxypoly (ethyleneglycol)-b-poly(ε-caprolactone-co-α-azido-ε-caprolactone) (mPEG-b-poly(εCL-co-αN3εCL)) as a precursor of reduction sensitive core-crosslinked micelles. The synthesized polymer was formulated as micelles using a dialysis method and loaded with the anti-inflammatory and anti-cancer drug metho- trexate (MTX). The micellar cores were subsequently crosslinked at their pendent azides by a redox- responsive bis(alkyne). The size distributions and morphology of the polymer micelles were assessed using dynamic light scattering (DLS) and transmission electron microscopy, and drug release assays were performed under simplified (serum free) physiological and reductive conditions. Cellular uptake studies in human breast cancer cells were performed using Oregon-green loaded core-crosslinked micelles. The MTX-loaded core-crosslinked micelles were assessed for their effects on metabolic activity in human breast cancer (MCF-7) cells by evaluating the reduction of the dye MTT 3-(4,5-dimethylthiazol-2-yl)-2,5- diphenyltetrazolium bromide. The apoptosis inducing potential of MTX-loaded core-crosslinked micelles was analysed using Hoechst/propidium iodide (PI) and annexin-V/PI assays. The data from these experi- ments indicated that drug release from these cross-linked micelles can be controlled and that the redox- responsive micelles are more effective carriers for MTX than non-crosslinked analogues and the free drug in the cell-lines tested. [less ▲]

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See detailUse of primary and secondary polyvinylamines for efficient gene transfection
Dréan, Mathilde; Debuigne, Antoine ULg; Gonçalves, Christine et al

in Biomacromolecules (2017), 18(2), 440-441

Gene transfection with polymeric carrier remains a challenge, particularly high transfection levels combined with low toxicity are hard to achieve. We herein revisit polyvinylamines, an old and neglected ... [more ▼]

Gene transfection with polymeric carrier remains a challenge, particularly high transfection levels combined with low toxicity are hard to achieve. We herein revisit polyvinylamines, an old and neglected family of cationic polymers. They can be readily obtained by controlled hydrolysis of polyvinylamides prepared through (controlled) radical polymerization. A series of tailor-made and well-defined polyvinylamines bearing primary amino groups, and poly(N- methylvinylamine) bearing secondary amines, were evaluated for the transfection of cells with pDNA as a function of their molar mass, molar mass distribution and degree of deacetylation. Unexpected high transfection levels, in combination with low cytotoxicity were recorded for both series. Surprisingly, a great impact of the molar mass was observed for the primary amine polyvinylamine series, whereas the results were mostly independent on molar mass or dispersity for the polymer bearing secondary amine. It was further established that a certain percentage of acetamide groups increased the transfection level, while maintaining low cytotoxicity. These results highlight for the first time the real potential of polyvinylamines as gene carriers, and make these polymers very attractive for further development in gene therapy. [less ▲]

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See detailPhotocleavable stabilizer for the preparation of PHEMA nanogels by dispersion polymerization in supercritical carbon dioxide
Alaimo, David; Grignard, Bruno ULg; Kuppan, Chandrasekar et al

in Polymer Chemistry (2017), 8(3), 581-591

A new photo-sensitive diblock copolymer composed of a hydrophilic sequence of poly(ethylene oxide) (PEO) linked to a CO2-philic sequence of poly(1H,1H,2H,2H-heptadecafluorodecyl acrylate) (PFDA) by a ... [more ▼]

A new photo-sensitive diblock copolymer composed of a hydrophilic sequence of poly(ethylene oxide) (PEO) linked to a CO2-philic sequence of poly(1H,1H,2H,2H-heptadecafluorodecyl acrylate) (PFDA) by a light sensitive o- nitrobenzyl group was successfully synthesized by RAFT polymerization and used as stabilizer for the free radical polymerization of 2-hydroxyethyl methacrylate (HEMA) in dispersion in ?,?,?-trifluorotoluene and supercritical carbon dioxide (scCO2). Thanks to this fluorinated stabilizer, well-defined particles of PHEMA down to 350 nm of diameter were produced in scCO2. Advantageously, the photocleavable group at the block junction of the stabilizer could be cleaved by exposing the particles to UV light so that the fluorinated block could be extracted in TFT or scCO2. As supported by X-ray photoelectron spectroscopy (XPS) analysis, up to 80 % of the fluorinated block of the stabilizer can be removed, leading to efficient swelling and dispersion of the resulting PHEMA nanogels in water. [less ▲]

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See detailHot-Melt Extrusion as a Continuous Manufacturing Process to Form Ternary Cyclodextrin Inclusion Complexes
Thiry, Justine ULg; Krier, Fabrice; Ratwatte, Shenelka et al

in European Journal of Pharmaceutical Sciences (2017), 96

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See detailReversible TAD chemistry as a convenient tool for the design of (re)processable PCL-based shape-memory materials
Defize, Thomas ULg; Riva, Raphaël ULg; Thomassin, Jean-Michel ULg et al

in Macromolecular Rapid Communications (2017), 38(1), 1600517

A chemically cross-linked but remarkably (re)processable shape-memory polymer (SMP) is designed by cross-linking poly(ε -caprolactone) (PCL) stars via the efficient triazolinedione click chemistry, based ... [more ▼]

A chemically cross-linked but remarkably (re)processable shape-memory polymer (SMP) is designed by cross-linking poly(ε -caprolactone) (PCL) stars via the efficient triazolinedione click chemistry, based on the very fast and reversible Alder– ene reaction of 1,2,4-triazoline-3,5-dione (TAD) with indole compounds. Typically, a six-arm star-shaped PCL function- alized by indole moieties at the chain ends is melt-blended with a bisfunctional TAD, directly resulting in a cross-linked PCL-based SMP without the need of post-curing treatment. As demonstrated by the stress relaxation measurement, the labile character of the TAD–indole adducts under stress allows for the solid-state plasticity reprocessing of the permanent shape at will by compression molding of the raw cross-linked material, while keeping excellent shape-memory properties. [less ▲]

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See detailPhotoreversibility and biocompatibility of polydimethylsiloxane-coumarin as adjustable intraocular lens material
Jellali, Rachid; Bertrand, Virginie ULg; Alexandre, Michaël et al

in Macromolecular Bioscience (2017)

Polydimethylsiloxane (PDMS) constitutes an interesting material for a variety of biomed- ical applications, especially as intraocular lenses (IOLs), for its excellent transparency. In this work, a ... [more ▼]

Polydimethylsiloxane (PDMS) constitutes an interesting material for a variety of biomed- ical applications, especially as intraocular lenses (IOLs), for its excellent transparency. In this work, a photoreversible PDMS-coumarin network, whose shape and properties can be adjusted postoperatively in a noninvasive manner, is developed. The synthesis of PDMS-cou- marin is achieved by amidation of a coumarin acid chloride derivative with amine-function- alized PDMSs. Under exposure of λ > 300 nm, these polymers can be cured by dimerization of coumarin. The cured polymers can be uncrosslinked via photocleavage of cyclobutane dimers upon illumination at λ < 290 nm. The diffusion of linear PDMSs in a crosslinked network and the controlled shape modification are studied, which demonstrate that these polymers are good candidates for adjustable IOL application. IOL disks prepared from these materials show high hydrophobicity and good transparency. In vitro cytotoxicity, lens epithelial cell adhesion assays, and rabbit host reaction against implanted disks demonstrate the biocompatibility of the polymer. [less ▲]

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See detailIn vitro evaluation of biocompatibility of uncoated thermally reduced graphene and carbon nanotube-loaded PVDF membranes with adult neural stem cell-derived neurons and glia
Defteralı, Çağla; Verdejo, Raquel; Majeed, Shahid et al

in Frontiers in Bioengineering and Biotechnology (2016), 4(n° 64),

Graphene, graphene-based nanomaterials (GBNs), and carbon nanotubes (CNTs) are being investigated as potential substrates for the growth of neural cells. However, in most in vitro studies, the cells were ... [more ▼]

Graphene, graphene-based nanomaterials (GBNs), and carbon nanotubes (CNTs) are being investigated as potential substrates for the growth of neural cells. However, in most in vitro studies, the cells were seeded on these materials coated with various proteins implying that the observed effects on the cells could not solely be attributed to the GBN and CNT properties. Here, we studied the biocompatibility of uncoated thermally reduced graphene (TRG) and poly(vinylidene fluoride) (PVDF) membranes loaded with multi-walled CNTs (MWCNTs) using neural stem cells isolated from the adult mouse olfactory bulb (termed aOBSCs). When aOBSCs were induced to differentiate on coverslips treated with TRG or control materials (polyethyleneimine-PEI and polyornithine plus fibronectin- PLO/F) in a serum-free medium, neurons, astrocytes, and oligodendrocytes were generated in all conditions, indicating that TRG permits the multi-lineage differentiation of aOBSCs. However, the total number of cells was reduced on both PEI and TRG. In a serum-containing medium, aOBSC-derived neurons and oligodendrocytes grown on TRG were more numerous than in controls; the neurons developed synaptic boutons and oligodendrocytes were more branched. In contrast, neurons growing on PVDF membranes had reduced neurite branching, and on MWCNTs-loaded membranes oligodendrocytes were lower in numbers than in controls. Overall, these findings indicate that uncoated TRG may be biocompatible with the generation, differentiation, and maturation of aOBSC-derived neurons and glial cells, implying a potential use for TRG to study functional neuronal networks. [less ▲]

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See detailPolyphosphoesters: new trends in synthesis and drug delivery applications
Ergül, Zeynep ULg; Jérôme, Christine ULg

in Macromolecular Bioscience (2016), 16(12), 1745-1761

Polymers with repeating phosphoester linkages in the backbone are biodegradable materials that emerge as a promising class of novel biomaterials, especially in the field of drug delivery systems. In ... [more ▼]

Polymers with repeating phosphoester linkages in the backbone are biodegradable materials that emerge as a promising class of novel biomaterials, especially in the field of drug delivery systems. In contrast to aliphatic polyesters, the pentavalency of the phosphorus atom offers a large diversity of structures and as a consequence a wide range of properties for these mate- rials. In this paper, it is focused on the synthesis of well-defined polyphosphoesters (PPEs) by organocatalyzed ring-opening polymerization, improving the functionalities by combination with click reactions, degrada- tion of functional PPEs and their cytotoxicity, and inputs for applications in drug delivery. [less ▲]

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See detailProtein encapsulation and release from PEO-b-polyphosphoester templated calcium carbonate particles
Ergül, Zeynep ULg; Cordonnier, Thomas; Debuigne, Antoine ULg et al

in International Journal of Pharmaceutics (2016), 513

Calcium carbonate particles are promising candidates as proteins carriers for their controlled delivery in the body. The present paper aims at investigating the protein encapsulation by in situ ... [more ▼]

Calcium carbonate particles are promising candidates as proteins carriers for their controlled delivery in the body. The present paper aims at investigating the protein encapsulation by in situ precipitation of calcium carbonate particles prepared by a process based on supercritical CO2 and using a new type of degradable well-defined double hydrophilic block copolymers composed of poly(ethylene oxide) and polyphosphoester blocks acting as templating agent for the calcium carbonate. For this study, lysozyme was chosen as a model for therapeutic protein for its availability and ease of detection. It was found that by this green process, loading into the CaCO3 microparticles with a diameter about 2 mm can be obtained as determined by scanning electron microscopy. A protein loading up to 6.5% active lysozyme was measured by a specific bioassay (Micrococcus lysodeikticus). By encapsulating fluorescent-labelled lysozyme (lysozyme-FITC), the confocal microscopy images confirmed its encapsulation and suggested a core–shell distribution of lysozyme into CaCO3, leading to a release profile reaching a steady state at 59% of release after 90 min. [less ▲]

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See detailHot-Melt Extrusion as a Continuous Manufacturing Process to Form Ternary Cyclodextrin Inclusion Complexes
Thiry, Justine ULg; Krier, Fabrice; Ratwatte, Shenelka et al

Poster (2016, November 16)

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See detailPolyhydroxyurethane hydrogels: synthesis and characterizations
Gennen, Sandro ULg; Grignard, Bruno ULg; Thomassin, Jean-Michel ULg et al

in European Polymer Journal (2016), 84

Hydrogels based on polyurethane (PU) are promising (bio-) materials because of their bio- compatibility, biodegradation and excellent mechanical properties. In this publication, polyurethane hydrogels ... [more ▼]

Hydrogels based on polyurethane (PU) are promising (bio-) materials because of their bio- compatibility, biodegradation and excellent mechanical properties. In this publication, polyurethane hydrogels were produced for the first time by a non-isocyanate route by solvent-free step-growth copolymerization between a CO2-sourced hydrophilic polyethy- lene glycol bi-cyclic carbonate with diamines in the presence of a cross-linker. Kinetic of poly(hydroxyurethane) (PHU) synthesis was monitored by ATR-IR and the chemical cross-linking was confirmed by rheology and gel contents measurements. Hydrogels were obtained by immersion of PHUs in water and the influence of the diamine/cross-linker ratio and the nature of diamine on the water swelling and compression properties (compression modulus, strain and stress at break) of PHU hydrogels was evaluated. Additionally, the compression properties of the hydrogels were improved by the addition of Montmorillonite as nanofiller in the PHU formulation. This work opens new application fields for CO2-sourced PHUs. [less ▲]

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See detailSurface- and redox-active multifunctional polyphenol-derived poly(ionic liquid)s: controlled synthesis and characterization
Patil, Nagaraj ULg; Cordella, Daniela; Aqil, Abdelhafid ULg et al

in Macromolecules (2016), 49(20), 7676-7691

Combining the redox activity and remarkable adhesion propensity of polyphenols (such as catechol or pyrogallol) with the numerous tunable properties of poly(ionic liquid)s (PILs) is an attractive route to ... [more ▼]

Combining the redox activity and remarkable adhesion propensity of polyphenols (such as catechol or pyrogallol) with the numerous tunable properties of poly(ionic liquid)s (PILs) is an attractive route to design inventive multifunctional macro-molecular platforms. In this contribution, we describe the first synthesis of a novel family of structurally well-defined PILs functionalized with catechol/pyrogallol/phenol pendants by organometallic-mediated radical polymerization (OMRP) using an alkyl−cobalt(III) complex as initiator and mediating agent. The living character of the chains is also exploited to produce di-and triblock PILs, and the facile counteranion exchange reactions afforded a library of PILs-bearing free phenol/catechol/pyrogallol moieties. Electrochemical investigations of catechol/pyrogallol-derived PILs in aqueous medium demonstrated the characteristic catechol to o-quinone transformations, whereas, quasi-reversible doping/undoping with supporting electrolyte cations (Li + /tetrabutylammonium +) has been observed in organic media, suggesting a bright future for this new family of redox-active PILs as cathode material for secondary energy storage devices. Also, pendant catechol/pyrogallol groups mediated sustained anchoring onto the gold surface conferred PILs properties to the interface. As a proof-of-concept, both the adsorption and inhibition of proteins on polymer modified surfaces have been demonstrated in real time using the quartz crystal microbalance with dissipation technique. The exquisite physicochemical tunability of these innovative surface-and redox-active PILs makes them excellent candidates for a broad range of potential applications, including " smart surfaces " and electrochemical energy storage devices. [less ▲]

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