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Title: Self-assembly of hydrophilic homopolymers: a matter of RAFT end groups
Authors: Du, Jianzhong
Willcock, Helen
Patterson, Joseph P.
Portman, Ian
O'Reilly, Rachel K.
Keywords: Polymers
Issue Date: 2011
Publisher: © Wiley-VCH
Citation: DU, J. ... et al., 2011. Self-assembly of hydrophilic homopolymers: a matter of RAFT end groups. Small, 7 (14), pp.2070-2080.
Abstract: Unusual self-assembly behavior is observed for a range of hydrophilic homopolymers. This self-assembly behavior is contrary to the expected behavior of such hydrophilic polymers and instead mimics more commonly reported amphiphilic block copolymers. It is proposed that the unique combination of hydrophobic end groups at both the α and Ω chain end accounts for this unusual self-assembly behavior. Complex internal polymer micelles are spontaneously formed when hydrophilic homopolymer polyelectrolytes and neutral polymers (with a weight fraction of the hydrophobic end groups <10 wt%) are directly dissolved in water. The homopolymers, poly[2-(diethylamino)ethyl methacrylate], poly(N-isopropylacrylamide), and poly(ethoxyethylacrylate) are synthesized by reversible addition-fragmentation chain-transfer (RAFT) polymerization using S′-1-dodecyl-(S′)-(α,α′- dimethyl-α″-acetic acid) trithiocarbonate (DDMAT) and its derivatives as chain transfer agents (CTAs). A range of polyelectrolyte homopolymers with different terminal groups are designed and synthesized, which under acidic aqueous solution direct the self-assembly to form well-defined nanostructures. This assembly behavior was also observed for neutral polymers, and it was determined that the structure of the hydrophobic end groups (and thus choice of RAFT CTA) are very important in facilitating this unusual self-assembly behavior of hydrophilic homopolymers. It is proposed that the functionality of commonly used CTAs such as DDMAT, can affect the solution association of the resultant homopolymers and can in fact afford ABA′ type polymers, which can undergo self-assembly to form higher-order nanostructures. © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Description: This is the peer reviewed version of the following article: DU, J. ... et al., 2011. Self-assembly of hydrophilic homopolymers: a matter of RAFT end groups. Small, 7 (14), pp.2070-2080, which has been published in final form at: http://dx.doi.org/10.1002/smll.201100382. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving.
Sponsor: The Leverhulme Trust is thanked for a post-doctoral fellowship for J.D. The EPSRC and Royal Society are thanked for support for R.K.O.R. The GPC used in this research was ... part-funded by the European Regional Development Fund (ERDF).
Version: Accepted for publication
DOI: 10.1002/smll.201100382
URI: https://dspace.lboro.ac.uk/2134/22891
Publisher Link: http://dx.doi.org/10.1002/smll.201100382
ISSN: 1613-6810
Appears in Collections:Published Articles (Materials)

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