Du, Jianzhong, Willcock, Helen, Patterson, Joseph P., Portman, Ian J. and O'Reilly, Rachel K.. (2011) Self-assembly of hydrophilic homopolymers : a matter of RAFT end groups. Small, Vol.7 (No.14). pp. 2070-2080. ISSN 1613-6810

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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 alpha and omega 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')-(alpha,alpha'-dimethyl-alpha ''-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.

Item Type:	Journal Article
Subjects:	Q Science > QD Chemistry
Divisions:	Faculty of Science > Chemistry
Library of Congress Subject Headings (LCSH):	Polymerization, Water-soluble polymers, Block copolymers, Diblock copolymers, Self-assembly (Chemistry)
Journal or Publication Title:	Small
Publisher:	Wiley - V C H Verlag GmbH & Co. KGaA
ISSN:	1613-6810
Date:	18 July 2011
Volume:	Vol.7
Number:	No.14
Page Range:	pp. 2070-2080
Identification Number:	10.1002/smll.201100382
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
Funder:	Engineering and Physical Sciences Research Council (EPSRC), Leverhulme Trust (LT), Royal Society (Great Britain)
URI:	http://wrap.warwick.ac.uk/id/eprint/38598

Data sourced from Thomson Reuters' Web of Knowledge

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