Self-healing metal-ligand polymeric materials

A method of making a self-healing polymeric material, the method comprising:

• mixing a polymer precursor, a precursor comprising a transition metal, and water together to form a mixture of a polymer comprising poly(vinyl alcohol) (PVA) having one or more ligands with at least one transition metal ion coordination site comprising hydroxy groups and a transition metal ion distributed in the polymer;
• freezing the mixture;
• and
• thawing the mixture, so as to form a self-healing material comprising a hydrogel polymer network having the transition metal ion distributed therein, wherein the one or more ligands with at least one transition metal ion coordination site comprising hydroxy groups of the hydrogel polymer network reacts with the transition metal ion to form a reversible coordination bond, wherein a first complex is defined for the transition metal ion and the transition metal ion coordination site, and a second complex is defined for the transition metal ion and water, wherein a ratio of the first complex to the second complex is greater than or equal to about 1:1 and less than or equal to about 5:1, and wherein the self-healing material is capable of self-healing a mechanical crack or cut in less than or equal to about 30 minutes at ambient conditions in an absence of external stimuli.