Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability using Asymmetrically Distributed Carboxyl-Fe3+Coordination Interactions

Recently,numerous mechanically robust synthetic hydrogels have been created.However,unlike natural loading-bearing materials such as cartilages and muscles,most hydrogels have inherently contradictory requirements,obstructing the design of hydrogels with characteristics of robustness and rapid self-recoverability.Herein,we present a facile strategy for constructing mechanically robust and rapidly self-recoverable hydrogels.The linear poly(acrylamide-co-itaconic acid)chains crosslink via coordination bonds and minimal chemical crosslinkers to form the hydrogel network.Such design endows the coordination interactions to be asymmetrically distributed.Under deformation,the coordination interactions exhibit a reversible dissociation-and-reorganization property,demonstrating a new mechanism for energy dissipation and stress redistribution.Thus,the hydrogels possess tensile strength up to 12.5 MPa and toughness up to 28.2 MJ/m3.Moreover,the inherent dynamic nature of the coordination bonds imparts these hydrogels with stretch rate-and temperature-dependent mechanical behavior as well as excellent self-recovery performance.The method employed in this study is universal and is applicable to other polymers with load-bearing yet rapid recovery conditions.This study will facilitate diverse applications of most metallosupramolecular hydrogels.