Glassy polymers are generally stiff and strong yet have limited extensibility¹. By swelling with solvent, glassy polymers can become gels that are soft and weak yet have enhanced extensibility^1,2,3. The marked changes in properties arise from the solvent increasing free volume between chains while weakening polymer–polymer interactions. Here we show that solvating polar polymers with ionic liquids (that is, ionogels^4,5) at appropriate concentrations can produce a unique class of materials called glassy gels with desirable properties of both glasses and gels. The ionic liquid increases free volume and therefore extensibility despite the absence of conventional solvent (for example, water). Yet, the ionic liquid forms strong and abundant non-covalent crosslinks between polymer chains to render a stiff, tough, glassy, and homogeneous network (that is, no phase separation)⁶, at room temperature. Despite being more than 54 wt% liquid, the glassy gels exhibit enormous fracture strength (42 MPa), toughness (110 MJ m⁻³), yield strength (73 MPa) and Young’s modulus (1 GPa). These values are similar to those of thermoplastics such as polyethylene, yet unlike thermoplastics, the glassy gels can be deformed up to 670% strain with full and rapid recovery on heating. These transparent materials form by a one-step polymerization and have impressive adhesive, self-healing and shape-memory properties.

玻璃状聚合物通常坚硬且坚固，但延展性有限 ¹ 。通过用溶剂溶胀，玻璃状聚合物可以变成柔软且脆弱的凝胶，但具有增强的延展性 ^1,2,3 。性能的显着变化是由于溶剂增加了链间的自由体积，同时削弱了聚合物与聚合物之间的相互作用。在这里，我们表明，用适当浓度的离子液体（即离子凝胶 ^4,5 ）溶解极性聚合物可以产生一类独特的材料，称为玻璃凝胶，具有玻璃和凝胶的理想特性。尽管不存在常规溶剂（例如水），离子液体仍增加了自由体积并因此增加了延展性。然而，离子液体在室温下在聚合物链之间形成牢固且丰富的非共价交联，从而形成坚硬、坚韧、玻璃状且均匀的网络（即无相分离） ⁶ 。尽管液体含量超过 54 wt%，玻璃状凝胶仍表现出巨大的断裂强度（42 MPa）、韧性（110 MJ m ⁻³ ）、屈服强度（73 MPa）和杨氏模量（1 GPa）。这些值与聚乙烯等热塑性塑料的值相似，但与热塑性塑料不同的是，玻璃状凝胶可变形高达 670% 的应变，并在加热时完全快速恢复。这些透明材料通过一步聚合形成，具有令人印象深刻的粘合、自修复和形状记忆特性。