Recently, we have constructed a high strength and thermoplastic supramolecular poly(N-acryloyl glycinamide) (PNAGA) hydrogel which can be developed as printable bioinks. However, the PNAGA hydrogel is low in stiffness and toughness, potentially limiting its application as load-bearing soft tissue scaffolds. In this work, we fabricate a supramolecular polymer double-network hydrogel based on hydrogen bonding crosslinked PNAGA and Fe³⁺-coordination crosslinked sodium carboxymethyl cellulose (CMC). The combined hydrogen bonding and ionic crosslinks contribute to high-strength nonswellable PNAGA/CMC-Fe hydrogels (Tensile strength of 2.9 MPa and compressive strength of 7.3 MPa at 80% strain without fracture) and stiffness (Young's modulus of 1.2 MPa and compressive modulus of 1.5 MPa). Furthermore, these reversible double physical crosslinks enable the PNAGA/CMC-Fe hydrogels to dissipate energy efficiently with a high toughness (12.3 MJ m⁻³) and tear energy (3700 J m⁻²), meanwhile imparting self-recoverability, anti-fatigue ability and self-healability to the network. This cytocompatible supramolecular polymer double network hydrogel with excellent multifaceted mechanical performances are promising to exploited as load-bearing soft tissue engineering scaffolds.

最近，我们已经构建了一种高强度的热塑性超分子聚N-丙烯酰基甘氨酰胺（PNAGA）水凝胶，可以将其开发为可印刷的生物墨水。但是，PNAGA水凝胶的刚度和韧性低，可能限制其作为承重的软组织支架的应用。在这项工作中，我们基于氢键交联的PNAGA和Fe ³⁺制备超分子聚合物双网络水凝胶-配位交联的羧甲基纤维素钠（CMC）。结合的氢键和离子交联键有助于形成高强度的非膨胀PNAGA / CMC-Fe水凝胶（2.9 MPa的拉伸强度，在80％应变下无断裂的抗压强度为7.3 MPa）和刚度（1.2 MPa的杨氏模量和1.5 MPa）。此外，这些可逆的双重物理交联使PNAGA / CMC-Fe水凝胶能够以高韧性（12.3 MJ m ^-3）和撕裂能（3700 J m ^-2）有效地耗散能量），同时赋予网络自我恢复能力，抗疲劳能力和自我修复能力。这种具有优异多方面机械性能的细胞相容性超分子聚合物双网络水凝胶有望用作承重的软组织工程支架。