In situ reduction and self-alignment of reduced graphene oxide/poly(vinylidene fluoride) composite films: Toward high dielectric constant and suppressed loss

• A fine dispersion and high degree of orientation of rGO nanofillers built. • GO nanosheets can be reduced in situ meanwhile self-align. • A better balance between dielectric permittivity and loss has been achieved. • The film can obtain electoral energy during the deformation/recovery process. In this work, we have successfully controlled the morphology and orientation of two-dimensional (2D) conductive filler reduced graphene oxide (rGO) via using ultra-thin film superimposed hot pressing method to obtain a novel poly(vinylidene fluoride) (PVDF) based composite films. Herein, GO nanosheets can be reduced in situ meanwhile self-align without any external force, resulting in fine dispersion and a high degree of orientation of rGO nanofillers, thereby endowing rGO/PVDF composite a well-balanced dielectric constant and loss. Accordingly, we can effectively obtain electrical energy from the rGO/PVDF nanocomposite generator during the film deformation/recovery process with this special oriented structure. Therefore, this work provides a method to achieve outstanding dielectric composites with well-arranged rGO for outstanding applications in energy harvesting and realizing self-powered electronics.