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Highly Tunable Nanostructures in a Doubly pH-Responsive Pentablock Terpolymer in Solution and in Thin Films

  • Multiblock copolymers with charged blocks are complex systems that show great potential for enhancing the structural control of block copolymers. A pentablock terpolymer PMMA-b-PDMAEMA-b-P2VP-b-PDMAEMA-b-PMMA is investigated. It contains two types of midblocks, which are weak cationic polyelectrolytes, namely poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and poly(2-vinylpyridine) (P2VP). Furthermore, these are end-capped with short hydrophobic poly(methyl methacrylate) (PMMA) blocks in dilute aqueous solution and thin films. The self-assembly behavior depends on the degrees of ionization α of the P2VP and PDMAEMA blocks, which are altered in a wide range by varying the pH value. High degrees of ionization of both blocks prevent structure formation, whereas microphase-separated nanostructures form for a partially charged and uncharged state. While in solutions, the nanostructure formation is governed by the dependence of the P2VP block solubility of the and the flexibility of the PDMAEMA blocks on α, in thin films, the dependence of the segregation strength on α is key. Furthermore, the solution state plays a crucial role in the film formation during spin-coating. Overall, both the mixing behavior of the 3 types of blocks and the block sequence, governing the bridging behavior, result in strong variations of the nanostructures and their repeat distances.

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Document Type:Article
Author:Florian A. JungORCiD, Maximilian Schart, Lukas Bührend, Elisabeth Meidinger, Jia-Jhen Kang, Bart-Jan NiebuurORCiD, Sina Ariaee, Dmitry S. MolodenskiyORCiD, Dorthe Posselt, Heinz AmenitschORCiD, Constantinos TsitsilianisORCiD, Christine M. PapadakisORCiD
Parent Title (English):Advanced Functional Materials
First Page:2102905
Year of first Publication:2021
Release Date:2022/08/10
Tag:block polymers; dynamic light scattering; grazing-incidence; pH-responsive polymers; small-angle-x-ray-scattering
Impact:19.924 (2021)
Funding Information:Deutsche Forschungsgemeinschaft. Grant Number: PA 771/19-1; Danish Council for Independent Research. Grant Number: DFF 7014-00288; BMBF. Grant Number: 16QK10A; Natur og Univers, Det Frie Forskningsråd. Grant Number: DFF 7014-00288
DDC classes:500 Naturwissenschaften und Mathematik / 540 Chemie
Open Access:Open Access
Signature:INM 2021/064
Licence (German):License LogoCreative Commons - CC BY - Namensnennung 4.0 International