Journal
LANGMUIR
Volume 25, Issue 4, Pages 2046-2054Publisher
AMER CHEMICAL SOC
DOI: 10.1021/la803616d
Keywords
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Funding
- Project of the Chinese Academy of Sciences (CAS)
- National Natural Scientific Foundation of China (NNSFC) Projects [20534020, 20874092, 20674079, 50425310]
- Specialized Research Fund for the Doctoral Program of Higher Education (SRFDP)
- Program for Changjiang Scholars and Innovative Research Team in University (PCSIRT)
- The Natural Sciences and Engineering Research Council of Canada (NSERC)
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A well-defined ABC triblock copolymer, poly(2-(2-methoxyethoxy)ethyl methacrylate)-b-poly(2-(dimethylamino)ethyl methacrylate)-b-poly(2-(diethylamino)ethyl methacrylate) (PMEO(2)MA-b-PDMA-b-PDEA), was synthesized via sequential atom transfer radical polymerization using ethyl 2-bromoisobutyrate as the initiator. Reacting the triblock precursor with propargyl bromide in anhydrous tetrahydrofuran yielded PMEO(2)MA-b-P(DMA-co-QDMA)b-PDEA triblock copolymer with clickable moieties, where QDMA was quaternized DMA residues. PMEO(2)MAb-P(DMA-co-QDMA)-b-PDEA triblock copolymer exhibited schizophrenic micellization behavior in aqueous solution, forming three-layer onion-like PMEO(2)MA-core and PDEA-core micelles upon proper adjustment of the solution pH and temperature. For temperature-induced formation of PMEO(2)MA-core micelles at acidic pH, the critical micellization temperature can be tuned by incorporating oligo(ethylene glycol) methyl ether methacrylate (OEGMA; the mean degree of polymerization was 8-9) residues into the PMEO(2)MA block, shifting from 38 to 43 degrees C as the OEGMA contents varied in the range of 0-10 mol %. In both types of micelles, the inner shell layer consisted of the middle P(DMA-co-QDMA) segment. Subsequently, cross-linking with tetra(ethylene glycol) diazide via click chemistry in the presence of copper catalysts led to the facile preparation of two types of shell-cross-linked (SCL) micelles with inverted structures in purely aqueous solution. The cores and coronas of SCL micelles exhibited multiresponsive swelling/shrinking and collapse/aggregation behavior, respectively. To the best of our knowledge, this represents the first report of the fabrication of two types of SCL micelles with inverted structures from a single schizophrenic water-soluble triblock copolymer in purely aqueous solution.
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