Hydrogels with high sacrifice efficiency of sacrificial bonds and with high strength and toughness due to dense entanglements of polymer chains.

Introducing sacrificial bonds is a common method for increasing the toughness of hydrogels. Many sacrificial bonds have been extensively investigated, but the sacrifice efficiency has never been studied. In this study, polyacrylamide hydrogels with highly entangled polymer chains containing carboxyl-zirconium (-COO-Zr) sacrificial bonds are prepared to study the effect of polymer chain entanglement on the sacrificial bond efficiency. Unlike chemical crosslinking points, the dense physical entanglements do not affect the toughness (∼43 MJ/m) of hydrogels but significantly improve the tensile strength (by two times) and Young's modulus (by six times). Physical entanglements enable the chains to slide and adjust the network structure under stress, which enables more polymer chains and sacrificial bonds to participate in the deformation process. Therefore, dense entanglements will greatly improve the sacrifice efficiency. However, a high density of chemical crosslinking points will limit the improvement in the sacrifice efficiency, which is attributed to the sliding limitations because of physical entanglement. The highly entangled polyacrylamide hydrogels toughened by -COO-Zr have an excellent load-bearing capacity. This study provides a novel strategy for designing hydrogels with ultra-high strength and toughness, which paves the way for the development of many hydrogels used in engineering materials.