Reversibly Interlocked Macromolecule Networks with Enhanced Mechanical Properties and Wide pH Range of Underwater Self-Healability

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 the topological reorganization of two preformed cross-linked polymers containing reversible catechol–Fe3+ coordinate bonds and imine bonds and exhibit enhanced mechanical properties, superior underwater self-healing effect within a wide pH range, and water-assisted recycling ability through synergetic action between the reversible catechol–Fe3+ and imine bonds. At higher pH values, the catechol–Fe3+ coordinate bonds are responsible for self-healing, while the imine bonds maintain the stability of the materials. In neutral water, the imine bonds mainly account for self-healing, and hydrogen bonds and entanglements between the two networks prevent the material from collapsing. Under a lower pH value, intermolecular hydrogen bonds and entanglements contribute to self-healing. The outcomes of this work provide a new idea for developing robust multifunctional underwater self-healing materials.