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Reversible addition-fragmentation chain transfer synthesis of amidine-based, CO2-responsive homo and AB diblock (Co)polymers comprised of histamine and their gas-triggered self-assembly in water

Quek, JY, Roth, PJ, Evans, RA, Davis, TP and Lowe, AB (2013) Reversible addition-fragmentation chain transfer synthesis of amidine-based, CO2-responsive homo and AB diblock (Co)polymers comprised of histamine and their gas-triggered self-assembly in water JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY, 51 (2). pp. 394-404.

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Abstract

Well-defined homopolymers of pentafluorophenyl acrylate (PFPA) and AB diblock copolymers of N,N-dimethylacrylamide (DMA) and poly(ethylene glycol) methyl ether acrylate (PEGA) with PFPA were prepared by reversible addition–fragmentation chain transfer (RAFT) radical polymerization. Three PFPA homopolymers of different molecular weights were reacted with the commercially available amidine and guanidine species histamine (HIS) dihydrochloride and L-arginine methyl ester (ARG) dihydrochloride in the presence of S-methyl methanethiosulfonate to yield, quantitatively, the corresponding amidine and guanidinebased acrylamido homopolymers. Both the HIS and ARG homopolymers are known to reversibly bind CO2 with, in the case of the former, CO2 fixation being accompanied with a switch from a hydrophobic to hydrophilic state. The RAFT synthesis of PFPADMA and PEGA-PFPA diblock copolymers yielded well-defined materials with a range of molar compositions. These precursor materials were converted to the corresponding HIS and ARG block copolymers whose structure was confirmed using 1 H NMR spectroscopy. Employing a combination of dynamic light scattering and transmission electron microscopy, we demonstrate that the DMA-HIS and PEGA-HIS diblock copolymers are able to undergo reversible and cyclable self-directed assembly in aqueous media using CO2 and N2 as the triggers between fully hydrophilic and amphiphilic (assembled) states. For example, in the case of the 54:46 DMA-HIS diblock, aggregates with hydrodynamic diameters of about 40.0 nm are readily formed from the molecularly dissolved state.

Item Type: Article
Subjects : Chemistry
Authors :
AuthorsEmailORCID
Quek, JYUNSPECIFIEDUNSPECIFIED
Roth, PJUNSPECIFIEDUNSPECIFIED
Evans, RAUNSPECIFIEDUNSPECIFIED
Davis, TPUNSPECIFIEDUNSPECIFIED
Lowe, ABUNSPECIFIEDUNSPECIFIED
Date : 15 January 2013
Identification Number : 10.1002/pola.26397
Copyright Disclaimer : Copyright 2012 Wiley Periodicals, Inc.
Uncontrolled Keywords : Science & Technology, Physical Sciences, Polymer Science, POLYMER SCIENCE, amidine, gas responsive, histamine, micelles, reversible addition fragmentation chain transfer (RAFT), self-assembly, stimulus responsive, AQUEOUS-SOLUTION CHARACTERIZATION, LIVING RADICAL POLYMERIZATION, RAFT POLYMERIZATION, BLOCK-COPOLYMERS, CARBON-DIOXIDE, SOLUBLE (CO)POLYMERS, POLYMERS, IMIDAZOLE, POLYSTYRENE, FIXATION
Related URLs :
Depositing User : Symplectic Elements
Date Deposited : 26 May 2016 12:14
Last Modified : 26 May 2016 12:14
URI: http://epubs.surrey.ac.uk/id/eprint/810844

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