Self-healing polymers with microphase-separated structure are plagued with inferior self-healing efficiency at room temperature due to a lack of dynamic interactions in hard domains. Herein, we describe a novel strategy of multiphase active hydrogen bonds (H-bonds), toward realizing fast and efficient self-healing at room temperature, even under harsh conditions. The core conception is to incorporate thiourea moieties into microphase-separated polyurea network to form multistrength H-bonds, which destroy the crystallization of hard domains and, at the same time, insert the dynamic reversible H-bonds in both hard and soft segments, accounting for the surprisingly self-healing performances. The synthesized polymeric material, poly(dimethylsiloxane)–4,4′-methylenebis(phenyl isocyanate)–1,1′-thiocarbonyldiimidazole, completely recovers all of the mechanical properties within 4 h at room temperature after rupture. Significantly, self-healing process can also take place at low temperature (restoration with an 85% efficiency in 48 h at −20 °C) or in the water (restoration with a 95% efficiency in 4 h). Depending on the cleavage/reformation of multiphase H-bonds, the material exhibits unprecedented ultrastrechability and notch-insensitiveness. It can be stretched up to 31 500% without fracture and reach a notch-insensitive stretching of up to 18 000%. These exceptional characteristics inspired us to fabricate highly stretchable self-healable underwater conductor and protective self-healing film for suppressing shuttling of polysulfides and preventing crack propagation in S cathode, which provide the pathway for applications in underwater electronic devices or advanced Li–S batteries.

中文翻译：

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由电子应用的多相活性氢键构成的，对缺口不敏感，可超拉伸，高效的自修复超分子聚合物

由于在硬域中缺乏动态相互作用，具有微相分离结构的自修复聚合物在室温下的自修复效率较差。在这里，我们描述了一种新型的多相活性氢键（H键）策略，旨在在室温甚至苛刻条件下实现快速有效的自我修复。核心概念是将硫脲部分掺入微相分离的聚脲网络中以形成多强度氢键，该氢键破坏硬结构域的结晶，同时在硬链段和软链段中插入动态可逆氢键，令人惊讶的自我修复表演。合成的高分子材料，聚（二甲基硅氧烷）–4,4'-亚甲基双（苯基异氰酸酯）–1,1'-硫代羰基二咪唑，破裂后在室温下4小时内完全恢复所有机械性能。重要的是，自修复过程也可以在低温下（在-20°C下48小时内以85％的效率进行恢复）或在水中（4小时内95％的效率进行的恢复）进行。取决于多相氢键的裂解/重整，该材料表现出空前的超拉伸性和缺口不敏感性。它可以拉伸至31 500％，而不会断裂，并且对缺口不敏感的拉伸可达18 000％。这些非凡的特性启发我们制造出高度可拉伸的自修复水下导体和保护性自修复膜，以抑制多硫化物的穿梭并防止裂纹在S阴极中传播，