A Guiding Principle for Strengthening Crosslinked Polymers: Synthesis and Application of Mobility-Controlling Rotaxane Crosslinkers

Angew Chem Int Ed Engl. 2019 Feb 25;58(9):2765-2768. doi: 10.1002/anie.201813439. Epub 2019 Jan 25.

Abstract

Three component mobility controlling vinylic rotaxane crosslinkers with two radically polymerizable vinyl groups (RC_Rs) were synthesized to prove that the mobility of the components of the RC_Rs plays a crucial role in determining the properties of rotaxane-crosslinked polymers (RCPs). RC_Rs (R=H, Me, or Et) were obtained from living ring-opening polymerization. RCP_Et was prepared using RC_Et, which exhibits the lowest component mobility. The low component mobility is reflected in inferior mechanical strength and stretching ability in tensile stress tests compared to components with good (R=Me) and high (R=H) mobility. However, RCP_Et exhibited significantly higher stress and strain values than the corresponding covalently crosslinked polymers (CCP_Rs). These results indicate that a suitable component mobility substantially enhances the mechanical strength of RCPs. This behavior could serve as a guiding principle for the molecular design of advanced RCs.

Keywords: mechanical properties; polymers; rotaxanes; supramolecular chemistry; synthetic methods.