Authors
Zifan Zhang, Li Liu
Published in
Macromolecular rapid communications. Pages e70379. Jul 26, 2026. Epub Jul 26, 2026.
Abstract
Sliding elastomers (SE) based on polyrotaxane (PR) architectures exhibit exceptional mechanical toughness through the "pulley effect". However, side-chain crystallization in such solvent-free systems often compromises molecular mobility and the efficiency of the topological cross-links. In this study, a series of solvent-free sliding elastomers was developed by grafting amorphous poly(ε-caprolactone-co-δ-valerolactone) [P(CL-co-VL)] side chains that are amorphous at ambient conditions onto a hydroxypropylated polyrotaxane (HPR) backbone via ring-opening polymerization. Systematic investigations were conducted by varying the side-chain degrees of polymerization (DP = 13, 26, 52) and the cross-linking indices (r = [NCO]/[OH]). The amorphous nature of the random copolymeric side chains effectively suppressed crystallization, thereby facilitating the unhindered sliding motion of α-cyclodextrin rings along the PEG axis. Compared to traditional fixed covalent cross-linking initiated by hydroxypropyl β-cyclodextrin (HPCD), these solvent-free elastomers exhibited superior mechanical performance, achieving a tensile strength of 10.2 MPa and an exceptional elongation at break of 830%. It is demonstrated that the synergy between topological sliding cross-links and the amorphous side-chain design allows for precise tuning of mechanical responses and stress homogenization. This work provides a robust strategy for the fabrication of high-performance, solvent-free topological elastomers with an optimized "pulley effect" for advanced flexible applications.
PMID:
42502902
Bibliographic data and abstract were imported from PubMed on 26 Jul 2026.
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