Synthetic hydrogels have achieved great progress in mechanical performance. But it is still a challenge to combine adequate stiffness, strength, and toughness in a single hydrogel. Herein, ultra-stiff, strong, and tough hydrogels are prepared by constructing a network with dense, small but strong hydrophobic associations. A hydrophobic monomer, 2-aminoethyl methacrylate isopropyl carbamate (IMA), is used to form strong hydrophobic associations enhanced by hydrogen bonding due to its hydrophobic moiety-protected carbamate side group. Low-reactive hydrophilic acrylamide (AAm) is copolymered with IMA at different monomer ratios to tailor the density, size, and strength of hydrophobic associations. Finally, a homogeneous and compact network based on dense but small and strong hydrophobic associations is constructed, and the hydrogels show comprehensive mechanical performance with the compressive modulus ranging from 28 to 200 MPa, compressive stress (85% strain) > 100 MPa, and compressive toughness from 9 to 26 MJ m⁻³. These hydrogels also display good self-recovery and fatigue resistance due to these dynamic cross-links. These ultra-stiff, strong, and tough hydrogels show great potential as load-bearing materials in many fields.

中文翻译：

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基于低反应性亲水单体的小而强疏水缔合的超硬而坚韧的水凝胶

合成水凝胶在机械性能方面取得了很大进步。但在单一水凝胶中结合足够的刚度、强度和韧性仍然是一个挑战。在此，通过构建具有致密、小但强疏水缔合的网络来制备超硬、强韧的水凝胶。疏水性单体甲基丙烯酸 2-氨基乙酯氨基甲酸异丙酯 (IMA) 由于其疏水部分保护的氨基甲酸酯侧基，用于形成通过氢键增强的强疏水缔合。低反应性亲水性丙烯酰胺 (AAm) 与 IMA 以不同的单体比例共聚，以调整疏水缔合的密度、大小和强度。最后，构建了一个基于密集但小而强的疏水关联的均匀紧凑网络，^-3。由于这些动态交联，这些水凝胶还显示出良好的自我恢复和抗疲劳性。这些超硬、坚固、坚韧的水凝胶在许多领域显示出作为承重材料的巨大潜力。