Due to the multiple different properties in self-healing elastomers that are mutually exclusive based on the different and contradictory molecule chain structures, simultaneously achieving the ultrahigh mechanical performance and high durability of self-healing elastomers is a great challenge and the goal that has always been pursued. Herein, we report a novel strategy to fabricate a self-healing elastomer by introducing interlaced hydrogen bonds with superhigh binding energy. Distinguishing from the quadruple hydrogen bonds reported already, the interlaced hydrogen bond with a lower repulsive secondary interaction and higher binding energy is composed of two molecule units with different lengths and steric hindrance. Connected by the interlaced hydrogen bonds, a supramolecule interlocking network is formed to lock the polymer chains at room temperature, endowing the poly(urethane–urea) elastomer with an unprecedented ultrahigh strength (117.5 MPa, even higher than some plastics), the superhigh fracture energy (522.46 kJ m–2), and an excellent puncture resistance (puncture force reached 181.9 N). Moreover, the elastomers also exhibited excellent self-healing properties (healing efficiency up to 95.8%), high transparency (the average transmittance up to 91.0%), and good durability (including thermal decomposition resistance, thermal oxidation aging resistance, water resistance, and solvent resistance), providing a theoretical basis and technical reference in the development and broadening the application prospects of self-healing elastomers.
Xinyou He,Haozhe Qin,Junxiang Liu,Jiaqi Wang,Zhiming Xiao,Lei Ming,Tongchao Liu,Khalil Amine,Xing Ou
Gel polymers are regarded as a promising candidate electrolyte for lithium-metal quasi-solid-state batteries, primarily due to their high ionic conductivity and solid-liquid synergistic properties. However, challenges such as interfacial side reactions, limitations in Li + transport caused by interfacial issues, and leaching of transition metals from the cathode have yet to be effectively solved. Herein, a novel gel electrolyte modulation strategy based on electrostatic filler assembly is proposed to address the issues of ineffective capacity utilization and inadequate cycling stability of high-energy-density cathode materials in solid-state lithium-ion batteries. It constructs a 3D interpenetrating charge-bridge network that effectively tackles the phase-separation challenge between fillers and electrolytes at the molecular level. Meanwhile, the molecular interlocking structure effectively inhibits the electrolyte erosion. More critically, it optimizes and stabilizes the cathode-electrolyte interface film, which facilitates the conduction of Li⁺-ions through a size-sieving mechanism. Consequently, this strategy enables effective adaptation across diverse high-energy-density cathode materials with satisfactory capacity performance (170.4 mAh g −1 at 4.5 V/1 C for LiNi 0.6 Co 0.2 Mn 0.2 O 2 and 194.0 mAh g −1 at 4.3 V/1 C for LiNi 0.9 Co 0.08 Mn 0.02 O 2 ). This investigation offers a straightforward and effective reference for addressing the critical challenges of ionic transport and interface stabilization in the design of gel electrolytes.
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