Reversible Self-Assembly of Degradable Polymersomes with Upper Critical Solution Temperature in Water

Thomas Wolf, Timo Rheinberger, Johanna Simon, Frederik R. Wurm*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

29 Citations (Scopus)

Abstract

Temperature-induced self-assembly of block copolymers allows the formation of smart nanodimensional structures. Mostly, nondegradable lower critical solution temperature (LCST) segments are applied to prepare such dynamic aggregates. However, degradable upper critical phase separation (UCST) block copolymers that would allow the swelling or disassembly at elevated temperatures with eventual backbone hydrolysis have not been reported to date. We present the first well-defined degradable poly(phosphonate)s with adjustable UCST. The organocatalytic anionic ring-opening copolymerization of 2-alkyl-2-oxo-1,3,2-dioxaphospholanes provided functional polymers with excellent control over molecular weight and copolymer composition. The prepolymers were turned into thermoresponsive polymers by thiol-ene modification to introduce pendant carboxylic acids. By this means, non cell-toxic, degradable polymers exhibiting UCST behavior in water between 43 and 71 °C were produced. Block copolymers with PEG as a nonresponsive water-soluble block can self-assemble into well-defined polymersomes with narrow size distribution. Depending on the responsive block, these structures either swell or disassemble completely upon an increased temperature.

Original languageEnglish
Pages (from-to)11064-11072
Number of pages9
JournalJournal of the American Chemical Society
Volume139
Issue number32
DOIs
Publication statusPublished - 16 Aug 2017
Externally publishedYes

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