Quadruple H-Bonding and Polyrotaxanes Dual Cross-linking Supramolecular Elastomer for High Toughness and Self-healing Conductors.

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 %.

Cyclodextrins-Based Polyrotaxanes: From Functional Polymers to Applications in Electronics and Energy Storage Materials.

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.

Solution-Processable Conductive Composite Hydrogels with Multiple Synergetic Networks toward Wearable Pressure/Strain Sensors.

A biocompatible, flexible, yet robust conductive composite hydrogel (CCH) for wearable pressure/strain sensors has been achieved by an all-solution-based approach. The CCH is rationally constructed by in situ polymerization of aniline (An) monomers in the polyvinyl alcohol (PVA) matrix, followed by the cross-linking of PVA with glutaraldehyde (GA) as the cross-linker. The unique multiple synergetic networks in the CCH including strong chemical covalent bonds and abundance of weak physical cross-links, i.e., hydrogen bondings and electrostatic interactions, impart excellent mechanical strength (a fracture tensile strength of 1200 kPa), superior compressibility (ε = 80%@400 kPa), outstanding stretchability (a fracture strain of 670%), high sensitivity (0.62 kPa-1 at a pressure range of 0-1.0 kPa for pressure sensing and a gauge factor of 3.4 at a strain range of 0-300% for strain sensing, respectively), and prominent fatigue resistance (1500 cycling). As the flexible wearable sensor, the CCH is able to monitor different types of human motion and diagnostically distinguish speaking. As a proof of concept, a sensing device has been designed for the real-time detection of 2D distribution of weight or pressure, suggesting its promising potentials for electronic skin, human-machine interaction, and soft robot applications.