Self-assembly Strategies Driven by Supramolecular RAFT Polymerization: Pseudorotaxanes and Nanosheets

Abstract

This study explores the use of supramolecular RAFT polymerization for the efficient synthesis of pseudorotaxanes and functional nanosheets through the host-guest interaction between β-cyclodextrin (β-CD) and the chain transfer agent (CTA) S,S’-bis(α,α’-dimethylacetic acid) trithiocarbonate (BDAAT). The formation of the β-CD@BDAAT complex significantly improves the water solubility of the CTA, thereby increasing the polymerization rate for N,N-dimethylacrylamide (DMA) and generating well-defined pseudorotaxane structure. In the process of aqueous polymerization-induced self-assembly (PISA), this supramolecular approach enables the rapid fabrication of functional nanosheets, reducing the required time from one week to just 5 h. The non-covalent support provided by β-CD is crucial for stabilizing the layered nanosheet assembly, while host-guest competition experiments also demonstrate the tunability of the morphology of non-covalently assembled structures. This study highlights the versatility of supramolecular RAFT polymerization, offering a promising strategy for the rapid and efficient production of complex nanostructures in aqueous media.

Keywords

RAFT / Host-guest systems / Polymerization-induced self-assembly (PISA) / Supramolecular assembly / Functional nanosheets / Nanostructures

RIGHTS & PERMISSIONS

2025 SIOC, CAS, Shanghai, & WILEY-VCH GmbH