LAUSR

A novel strategy for developing homogeneous reversibly interlocking polymer networks (RILNs) with enhanced mechanical properties and underwater self-healing ability is proposed. The RILNs are prepared by topological reorganization of two preformed crosslinked polymers containing reversible catechol-Fe3+ coordinate bonds and imine bonds, respectively, and exhibit enhanced mechanical properties, superior underwater self-healing effect within a wide pH range, as well as water-assisted recycling ability through synergetic action between the reversible catechol-Fe3+ and imine bonds. At higher pH value, the catechol-Fe3+ coordinate bonds take responsible for self-healing, while the imine bonds maintain the stability of the material. In neutral water, the imine bonds mainly account for self-healing, and hydrogen bonds and entanglements between the two networks prevent the material from collapse. Under lower pH value, intermolecular hydrogen bonds and entanglements contribute to self-healing. The outcomes of this work provide a new idea for developing robust multi-functional underwater self-healing materials.