Highly Tunable Nanostructures in a Doubly pH‐Responsive Pentablock Terpolymer in Solution and in Thin Films
Highly Tunable Nanostructures in a Doubly pH‐Responsive Pentablock Terpolymer in Solution and in Thin Films
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溶液和薄膜中双 pH 响应性五嵌段三元共聚物中的高度可调纳米结构
DOI：
10.1002/adfm.202102905
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发表时间：
--
影响因子：
19
通讯作者：
C. M. Papadakis
中科院分区：
文献类型：
--
作者：
F. A. Jung;M. Schart;L. Bührend;E. Meidinger;J.-J. Kang;B.-J. Niebuur;S. Ariaee;D. D. Molodenskiy;D. Posselt;H. Amenitsch;C. Tsitsilianis;C. M. Papadakis
带电荷嵌段多嵌段共聚物是一种复杂体系，在增强嵌段共聚物的结构控制方面显示出巨大的潜力。研究了五嵌段聚甲基丙烯酸甲酯-B-PDMAEMA-B-P2 VP-B-PDMAEMA-B-PMMA。它含有两种类型的中间嵌段，它们是弱阳离子聚电解质，即聚（2-（二甲基氨基）乙基甲基丙烯酸酯）（PDMAEMA）和聚（2-乙烯基吡啶）（P2 VP）。此外，这些在稀水溶液和薄膜中用短疏水聚（甲基丙烯酸甲酯）（PMMA）嵌段封端。自组装行为取决于P2 VP和PDMAEMA嵌段的电离度α，其通过改变pH值在很大范围内改变。两种嵌段的高度电离防止结构形成，而微相分离的纳米结构形成部分带电和不带电状态。而在溶液中，纳米结构的形成取决于P2 VP嵌段的溶解度和PDMAEMA嵌段的柔性对α的依赖性，在薄膜中，偏析强度对α的依赖性是关键。此外，溶液状态在旋涂过程中的成膜过程中起着至关重要的作用。总的来说，这3种类型的嵌段的混合行为和控制桥接行为的嵌段序列都导致纳米结构及其重复距离的强烈变化。
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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