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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 detailInterpolymer radical coupling: A toolbox complementary to controlled radical polymerization
Debuigne, Antoine ULg; Hurtgen, Marie ULg; Detrembleur, Christophe ULg et al

in Progress in Polymer Science (2012), 37(7), 1004-1030

The current review focuses on the relevance and practical benefit of interpolymer radical coupling methods. The latter are developing rapidly and constitute a perfectly complementary macromolecular ... [more ▼]

The current review focuses on the relevance and practical benefit of interpolymer radical coupling methods. The latter are developing rapidly and constitute a perfectly complementary macromolecular engineering toolbox to the controlled radical polymerization techniques (CRP). Indeed, all structures formed by CRP are likely to be prone to radical coupling reactions, which multiply the available synthetic possibilities. Basically, the coupling systems can be divided in two main categories. The first one, including the atom transfer radical coupling (ATRC), silane radical atom abstraction (SRAA) and cobalt-mediated radical coupling (CMRC), relies on the recombination of macroradicals produced from a dormant species. The second one, including atom transfer nitroxide radical coupling (ATNRC), single electron transfer nitroxide radical coupling (SETNRC), enhanced spin capturing polymerization (ESCP) and nitrone/nitroso mediated radical coupling (NMRC), makes use of a radical scavenger in order to promote the conjugation of the polymer chains. More than a compilation of macromolecular engineering achievements, the present review additionally aims to emphasize the particularities, synthetic potential and present limitations of each system. [less ▲]

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See detailCathodic electrografting of acrylics: From fundamentals to functional coatings
Gabriel, Sabine ULg; Jérôme, Robert ULg; Jérôme, Christine ULg

in Progress in Polymer Science (2010), 35

Promoting permanent adhesion between so dissimilar materials as polymers and metals is a very challenging target and a severe brake to the implementation of many potential applications. However, synthetic ... [more ▼]

Promoting permanent adhesion between so dissimilar materials as polymers and metals is a very challenging target and a severe brake to the implementation of many potential applications. However, synthetic polymers can now be chemisorbed onto a variety of conducting surfaces by cathodic electrografting of acrylic monomers. The first part of this review will focus on the fundamental aspects of this emerging technology, thus from the historical discovery to experimental and theoretical developments, with the purpose to better comprehend the electrografting phenomenon. Once firmly established, this concept has been exploited in order to make polymeric coatings with specific functionality chemisorbed onto more diversified substrates in more convenient liquid media. This remarkable progress that largely relies on advanced controlled polymerization processes will be the topic of the second part of the review, with a special emphasis on the more recent development of smart coatings, particularly stimuli responsive coatings very well-suited to nanotechnologies. [less ▲]

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See detailOverview of cobalt-mediated radical polymerization: roots, state of the art and future prospects
Debuigne, Antoine ULg; Poli, Rinaldo; Jérôme, Christine ULg et al

in Progress in Polymer Science (2009), 34(3), 211-239

Controlled radical polymerization (CRP) techniques offer the opportunity to properly design polymer chains and adjust their chemical and physical properties. Among these techniques, cobalt-mediated ... [more ▼]

Controlled radical polymerization (CRP) techniques offer the opportunity to properly design polymer chains and adjust their chemical and physical properties. Among these techniques, cobalt-mediated radical polymerization (CMRP) distinguished itself by the high level of control imparted to the polymerization of acrylic and vinyl ester monomers, even for high molar masses. This article summarizes for the first time the advances in understanding and synthetic scope of CMRP since its discovery. Notably, the cobalt–carbon bond formation by dual contribution of reversible termination and degenerative chain transfer is discussed, as well as the impact of additives able to coordinate the metal. The potential of computational chemistry in the field of CMRP as a rationalization and predicting tool is also presented. These mechanistic considerations and achievements in macromolecular engineering will be discussed along with challenges and future prospects in order to assess the CMRP system as a whole. [less ▲]

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See detailIonic end-capping of (semi)telechelic polymers by mesogens: a novel route to liquid crystalline polymers
Gohy, Jean-François; Jérôme, Robert ULg

in Progress in Polymer Science (2001), 26(7), 1061-1099

A mesogenic cation has been associated with low molecular weight carboxylato- and sulfonato-(semi)telechelic polymers to form liquid crystalline halato(semi)telechelic polymers (LC H(S)TPs). Two methods ... [more ▼]

A mesogenic cation has been associated with low molecular weight carboxylato- and sulfonato-(semi)telechelic polymers to form liquid crystalline halato(semi)telechelic polymers (LC H(S)TPs). Two methods have been used to end-cap the linear polymer chains at one (or both) end(s) by a mesogen through ionic bonding. The first method relies on the ion-exchange reaction between the metal counterion of halato(semi)telechelic polymers and an ionic mesogen. The second method is based on the proton-transfer from a sulfonic or carboxylic acid end-group to a tertiary aliphatic amine, this approach being controlled by the relative pKa's of the acid and basic groups. The resulting materials have been characterized by differential scanning calorimetry (DSC), polarized optical microscopy (POM), small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS). On the basis of these experimental results, a model for the supramolecular organization of the LC H(S)TPs has been proposed. The final morphology results from the interplay of two competitive effects: the dipolar interaction of the ion-pairs known for multiplets formation and the propensity of the mesogenic moiety to form mesophases. The outcome of this competition depends on the mobility of the mesogenic counterion, i.e. on the strength of the dipolar interactions, the mobility of the polymer backbone and the mesogen/polymer ratio, which is controlled by the polymer molecular weight. A rod-like organization of the multiplets and a stretching of the polymer chains in the very close vicinity of the mesogenic core has been found in sulfonate polystyrenes, in agreement with the Eisenberg, Hird and Moore model for ionomers. The thickness of this region of restricted mobility has been estimated to 1 nm, which is the order of magnitude of the persistence length of polystyrene. Finally, LC H(S)TPs have been tested as interfacial agents in polystyrene/liquid crystal dispersions. The dipolar interactions of the ion pairs are clearly favorable to the additive localization at the polymer/LC interface. The higher polarity of the ammonium sulfonate pairs compared to the parent ammonium carboxylate ion pairs accordingly accounts for a higher interfacial activity. [less ▲]

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See detailAnionic polymerization of methacrylic monomers: characterization of the propagating species
Zune, Catherine; Jérôme, Robert ULg

in Progress in Polymer Science (1999), 24(5), 631-664

Ligation of the anionic species responsible for the polymerization (LAP) of alkyl(meth)acrylates has much contributed to improve polymerization control. This ligated anionic polymerization has been ... [more ▼]

Ligation of the anionic species responsible for the polymerization (LAP) of alkyl(meth)acrylates has much contributed to improve polymerization control. This ligated anionic polymerization has been firstly studied by using model compounds, such as low molecular weight lithium ester enolates. Recently, effort has been devoted to the direct analysis of the species that propagate the anionic polymerization of (meth)acrylates. In addition to IR, multinuclear NMR spectroscopy has been very instrumental in the elucidation of the structure and aggregation of the active species and how these characteristic features are modified by the addition of various types of ligands. This substantial progress in the characterization of the polyalkyl(meth)acrylate anions, ligated or not, is reported in this review. [less ▲]

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See detailStrategies for compatibilization of polymer blends
Koning, Cor; Van Duin, Martin; Pagnoulle, Christophe et al

in Progress in Polymer Science (1998), 23(4), 707-757

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