Block Copolymers with Crystallizable Blocks: Synthesis, Self-Assembly and Applications

Dear Colleagues,

Block copolymers with crystallizable blocks have recently moved to the forefront of current research owing to their unique self-assembly behaviour and properties. New synthetic concepts give, for example, access to tetrablock copolymers with four crystalline blocks, bio-based thermoplastic elastomers (e.g., based on ABA triblock copolymers with hard poly(L-lactide) (PLLA) segments), and conjugated semi-crystalline block copolymers for photovoltaics and allow for new, exciting insights into the interplay between the microphase separation and crystallization controlling self-assembly in bulk (confined vs. break-out crystalliza­tion).

Concerning self-assembly in solution, the pioneering work of Manners and Winnik paved the way to a myriad of crystalline-core micellar structures and hierarchical super­structures that were not accessible before via self-assembly of fully amorphous block copolymers. In analogy to living polymerization, crystallization-driven self-assembly (CDSA) can be conducted in a living manner using small micellar fragments as seeds for the addition of unimers (molecularly dissolved block copolymers bearing a crystallizable block). This allows for the production of cylindrical micelles with defined length, length distribution, corona chemistries (block type or patchy corona), branched micelles, and micellar superstructures (e.g., two-dimensional (2D) lenticular platelets, scarf-shaped micelles, multidimensional micellar assemblies, and cross and “windmill”-like supermicelles). Moreover, amphiphilic crystalline-core micelles based on PLLA or corresponding stereo-complexes (e.g., PLLA/PDLA (poly(D-lactide)) show interesting potential for biomedical applications (controlled release and delivery of drugs). Use of the process termed polymerization-​induced crystallization-​driven self-​assembly (PI-​CDSA) enables the one-​pot production of a highly concentrated dispersion of crystalline-core cylindrical micelles.

This Special Issue aims to present a collection of articles describing new developments in the synthesis and self-assembly (bulk and solution) of block copolymers with crystallizable blocks. It also aims to address emerging applications for these exciting materials.

Dr. Holger Schmalz
Guest Editor

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