High‐Strength and High‐Toughness Supramolecular Materials for Self‐Healing Triboelectric Nanogenerator

The development of self-healing materials provides a new opportunity and challenge for advancing triboelectric nanogenerators (TENGs). However, the low strength and low toughness of self-healing triboelectric materials often result in the deformation or breakage of TENG under high mechanical loads, thereby limiting their potential applications. Herein, a new strategy for fabricating self-healing triboelectric materials is reported, which introduces cross-linking networks with hydrogen bonds and metal coordination bonds. The desired high performance can be achieved by simply adjusting the molar ratio of the metal to the ligand. When the molar ratio is 1:2, the tensile strength, toughness, and elongation at break of the material reached 13.7 MPa, 76.9 MJ m^-3, and 1321%, respectively. Furthermore, its self-healing efficiency can reach 74% at 70 °C in 6 h. Working in contact-separation mode, the electrical output can reach 164 V, 18.2 µA, 57.5 nC, with a maximum power density of 2.54 W m^-2. Notably, even if it is sheared, the electrical output performances of TENG can be completely recovered to the original state. In addition, the developed TENG exhibits excellent output stability over 10 000 contact separation cycles. This study presents a promising approach for the development of stretchable smart generators.