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In this study, we examine how the self-assembly of crystalline-coil block copolymers in solution can be influenced by small changes in the chemical structure of the corona-forming block. Three samples of poly(ferrocenyldimethylsilane)-block-poly(2-vinylpyridine) that form long fiber-like micelles uniform in width in 2-propanol, were treated with methyl iodide to convert a small fraction (0.1% to 6%) of the pyridines to methylpyridinium groups. When these partially quaternized samples (PFS-b-P2VPQ) were subjected to the same self-assembly protocol, very different structures were obtained. For PFS36-b-P2VP502Q, the presence of positive charges led to the formation of much shorter rod-like micelles. In contrast, for PFS17-b-P2VP170Q and PFS30-b-P2VP300Q, complex platelet structures were obtained. We explain the complexity of these structures in terms of a distribution of compositions, in which the polymer chains with the highest extent of methylation are the least soluble in 2-PrOH and the first to associate...

How a Small Modification of the Corona-Forming Block Redirects the Self-Assembly of Crystalline–Coil Block Copolymers in Solution