One-pot mechanochemical assembly of lignocellulose nanofiber/graphite nanocomposites for wearable electronic devices

Carbon nanomaterials are indispensable in electronic applications because of their superior electronic properties and mechanical performances. Assembling carbon nanomaterials in a facile and environmentally benign manner, on the other hand, remains a challenge. In this study, a green one-pot co-ball milling strategy was developed for fabricating water-dispersible lignocellulose nanofiber-decorated graphite-flake nanocomposites ([email protected]), followed by the preparation of versatile hydrogels by mixing [email protected] with a polyvinyl alcohol–borax matrix comprising a binary ethylene glycol/water solvent system. Because of the intrinsic conductivity and abundant functional groups of [email protected], these flake-shaped nanocomposites were evenly dispersed and dynamically crosslinked with hydrogel matrix that perfectly integrates ultrastretchability (∼3500%), fast self-healing (30 s), self-adhesiveness, good conductivity (1.33 S/m), and high strain sensitivity (GF = 3.19 at 500%–1000%) in a single hydrogel. Furthermore, the hydrogel demonstrated outstanding anti-freezing (−23 °C) and long-term moisturizing properties (7 days). Importantly, the multifunctional hydrogel can be utilized to wirelessly monitor large and small human actions, as well as control a two-degree-of-freedom virtual robot arm. This study describes a facile and eco-friendly strategy for preparing carbon-based nanocomposites, which can be extended to wireless soft electrical devices and intelligent robotics.