A novel type of polymeric material with tunable mechanical properties is fabricated from polymers and small molecules that can form hydrogen‐bonded intermolecular complexes (IMCs). In this work, poly(vinyl alcohol) (PVA)–glycerol hydrogels are first prepared, and then they are dried to form IMCs. The tensile strengths and moduli of IMCs decrease dramatically with increasing glycerol content, while the elongations increase gradually. The mechanical properties are comparable with or even superior to those of common engineering plastics and rubbers. The IMCs with high glycerol content also show excellent flexibility and cold‐resistance at subzero temperatures. Cyclic tensile and stress relaxation tests prove that there is an effective energy dissipation mechanism in IMCs and dynamic mechanical analysis confirms their physical crosslinking nature. FTIR and NMR characterizations prove the existence of hydrogen bonding between glycerol and PVA chains, which suppresses the crystallization of PVA from X‐ray diffraction measurement. These PVA–glycerol IMCs may find potential applications in barrier films, biomedical packaging, etc., in the future.

中文翻译：

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具有可调机械性能的氢键聚合物小分子复合物

一种新型的具有可调机械性能的聚合物材料是由可以形成氢键分子间复合物（IMC）的聚合物和小分子制造的。在这项工作中，首先准备了聚乙烯醇（PVA）-甘油水凝胶，然后将其干燥以形成IMC。随着甘油含量的增加，IMC的拉伸强度和模量急剧下降，而伸长率则逐渐增加。机械性能可与甚至优于普通工程塑料和橡胶。甘油含量高的IMC在零度以下温度下也显示出出色的柔韧性和耐寒性。循环拉伸和应力松弛测试证明，IMC中存在有效的能量耗散机制，动态力学分析证实了它们的物理交联性质。FTIR和NMR表征证明甘油和PVA链之间存在氢键，从而抑制了X射线衍射测量中PVA的结晶。这些PVA-甘油IMC将来可能会在阻隔膜，生物医学包装等方面发现潜在的应用。