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The concept of polyrotaxane comes from the rotaxane structure in the supramolecular field. It is a mechanically interlocked supramolecular assembly composed of linear polymer chains and cyclic molecules. Over recent decades, the synthesis and application of polyrotaxanes have seen remarkable growth. Particularly, cyclodextrin‐based polyrotaxanes have been extensively reported due to the low‐price raw materials, good biocompatibility, and ease of modification. Hence, it is also one of the most promising mechanically interlocking supramolecules for wide industrialization in the future. Polyrotaxanes are widely introduced into materials such as elastomers, hydrogels, and engineering polymers to improve their mechanical properties or impart functionality to the materials. In these materials, polyrotaxane acts as a slidable cross‐linker to dissipate energy through sliding or assist in dispersing stress concentration in the cross‐linked network, thereby enhancing the toughness of the materials. Further, the unique sliding‐ring effect of cyclodextrin‐based polyrotaxanes has pioneered advancements in stretchable electronics and energy storage materials. This includes their innovative use in stretchable conductive composite and binders for anodes, addressing critical challenges in these fields. In this mini‐review, our focus is to highlight the current progress and potential wider applications in the future, underlining their transformative impact across various domains of material science. [ABSTRACT FROM AUTHOR]

Ionic conductive soft materials for mimicking human skin are a promising topic since they can be thought of as a possible basis for biomimetic sensing. In pursuit of devices with a long working range and low signal delay, conductive materials with low hysteresis and good stretchability are highly demanded. To overcome the challenges of highly stretchable conductive materials with good resilience, herein a chemical design is proposed where polyrotaxanes act as topological cross‐linkers to enhance the stretchability by sliding‐induced reduced stress concentration while the compatible ionic liquid is introduced as a dispersant for low hysteresis. The obtained ionogels exhibit versatile properties more than low hysteresis (residual strain = 7%) and good stretchability (550%), and also anti‐fatigue, biocompatibility, and good adhesion. The low hysteresis is attributed to lower energy dissipation from the well‐dispersed polyrotaxanes by compatible ionic liquids. The mechanism provides a new insight in fabricating highly stretchable and low‐hysteresis slide‐ring materials. Furthermore, the conductivity of the ionogels and their responses to strains and temperatures are measured. Benefiting from the good conductivity and low hysteresis, the ionogel is applied to develop a wireless communication system to realize rapid human‐machine interactions. [ABSTRACT FROM AUTHOR]

Tough and self‐healable substrates can enable stretchable electronics long service life. However, for substrates, it still remains a challenge to achieve both high toughness and autonomous self‐healing ability at room temperature. Herein, a strategy by using the combined effects between quadruple H‐bonding and slidable cross‐links is proposed to solve the above issues in the elastomer. The elastomer exhibits high toughness (77.3 MJ m−3), fracture energy (≈127.2 kJ m−2), and good healing efficiency (91 %) at room temperature. The superior performance is ascribed to the inter and intra crosslinking structures of quadruple H‐bonding and polyrotaxanes in the dual crosslinking system. Strain‐induced crystallization of PEG in polyrotaxanes also contributes to the high fracture energy of the elastomers. Furthermore, based on the dual cross‐linked supramolecular elastomer, a highly stretchable and self‐healable electrode containing liquid metal is also fabricated, retaining resistance stability (0.16–0.26 Ω) even at the strain of 1600 %. [ABSTRACT FROM AUTHOR]

Tough and self‐healable substrates can enable stretchable electronics long service life. However, for substrates, it still remains a challenge to achieve both high toughness and autonomous self‐healing ability at room temperature. Herein, a strategy by using the combined effects between quadruple H‐bonding and slidable cross‐links is proposed to solve the above issues in the elastomer. The elastomer exhibits high toughness (77.3 MJ m−3), fracture energy (≈127.2 kJ m−2), and good healing efficiency (91 %) at room temperature. The superior performance is ascribed to the inter and intra crosslinking structures of quadruple H‐bonding and polyrotaxanes in the dual crosslinking system. Strain‐induced crystallization of PEG in polyrotaxanes also contributes to the high fracture energy of the elastomers. Furthermore, based on the dual cross‐linked supramolecular elastomer, a highly stretchable and self‐healable electrode containing liquid metal is also fabricated, retaining resistance stability (0.16–0.26 Ω) even at the strain of 1600 %. [ABSTRACT FROM AUTHOR]