Preparation of strong and tough conductive hydrogel based on Grafting, Fe3+-Catechol complexations and salting out for triboelectric nanogenerators

The development of a strong and tough conductive hydrogel capable of meeting the strict requirements of the electrode of a hydrogel-based triboelectric nanogenerator (H-TENG) remains an enormous challenge. Herein, a robust conductive polyvinyl alcohol (PVA) hydrogel is designed via a three-step method: (1) grafting with 3,4-dihydroxy benzaldehyde, (2) metal complexation using ferric chloride (FeCl3) and (3) salting-out using sodium citrate. The hydrogel contains robust crystalline PVA domains and reversible/high-density non-covalent interactions, such as hydrogen bonding, π–π interactions and Fe3+-catechol complexations. Benefiting from the crystalline domains, the hydrogel can resist external forces to the hydrogel network; meanwhile, the reversible/high-density of non-covalent interactions can impart gradual and persistent energy dissipation during deformation. The hydrogel possesses multiple cross-linked networks, with 6.47 MPa tensile stress, 1000 % strain, 35.24 MJ/m3 toughness and 37.59 kJ/m2 fracture energy. Furthermore, the inter-connected porous hydrogel has an ideal structure for ionic-conducing channels. The hydrogel is assembled into an H-TENG, which can generate open circuit voltage of ∼ 150 V, short-circuit current of ∼ 3.0 μA, with superb damage immunity. Subsequently, road traffic monitoring systems are innovatively developed and demonstrated by using the H-TENG. This study provides a novel strategy to prepare superiorly strong and tough hydrogels that can meet the high demand for H-TENGs.