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ABSTRACT: The supramolecular crosslinking of polymer chains in water by specific, directional and dynamic non-covalent interactions has led to the development of novel supramolecular polymeric hydrogels. These aqueous polymeric networks constitute an interesting class of soft materials exhibiting attractive properties such as stimuli-responsiveness and self-healing arising from their dynamic behaviour and that are crucial for a wide variety of emerging applications. We present here a critical review summarising the formation of dynamic polymeric networks through specific non-covalent interactions, with a particular emphasis on those systems based on host-guest complex formation, as well as the characterisation of their physical characteristics. Aqueous supramolecular chemistry has unlocked a versatile toolbox for the design and fine-tuning of the material properties of these hydrogels (264 references).
Chemical Society Reviews 08/2012; 41(18):6195-214. · 28.76 Impact Factor
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ABSTRACT: Smart materials: Metastable single-chain polymeric nanoparticles were prepared through stimuli-responsive and reversible intramolecular crosslinking of a single polymer chain in water. Functionalization of poly(N-hydroxyethylacrylamide) polymers with two complementary guests for cucurbit[8]uril (CB[8]), namely viologen and naphthalene, followed by addition of the macrocycle thus allowed for facile preparation of such nanoparticles.
Angewandte Chemie International Edition 03/2012; 51(17):4185-9. · 13.45 Impact Factor
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ABSTRACT: The synthesis of a supramolecular double hydrophilic block copolymer (DHBC) held together by cucurbit[8]uril (CB[8]) ternary complexation and its subsequent self-assembly into micelles is described. This system is responsive to multiple external triggers including temperature, pH and the addition of a competitive guest. The supramolecular block copolymer assembly consists of poly(N-isopropylacrylamide) (PNIPAAm) as a thermoresponsive block and poly(dimethylaminoethylmethacrylate) (PDMAEMA) as a pH-responsive block. Moreover, encapsulation and controlled drug release was demonstrated with this system using the chemotherapeutic drug doxorubicin (DOX). This triple stimuli-responsive DHBC micelle system represents an evolution over conventional double stimuli-responsive covalent diblock copolymer systems and displayed a significant reduction in the viability of HeLa cells upon triggered release of DOX from the supramolecular micellar nanocontainers.
Biomacromolecules 12/2011; 13(1):84-91. · 5.48 Impact Factor
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ABSTRACT: The chain end complexation of a functional PNIPAM by a cucurbit[8]uril-viologen complex causes a shift in its lower critical solution temperature (LCST) by over 5 °C. An instantaneous phase change of the thermally responsive polymer beyond its LCST can be induced by addition of the aqueous cucurbituril host-guest complex. Subsequent decomplexation upon addition of a competitive guest releases the PNIPAM terminus and triggers complete reversibility.
Chemical Communications 06/2011; 47(21):6000-2. · 6.17 Impact Factor
