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Flexible Hybrid Paper Made of Monolayer Co3O4 Microsphere Arrays on rGO/CNTs and Their Application in Electrochemical Capacitors

A facile one‐step hydrothermal method is developed for large‐scale production of well‐designed flexible and free‐standing Co3O4/reduced graphene oxide (rGO)/carbon nanotubes (CNTs) hybrid paper as an electrode for electrochemical capacitors. Densely packed unique Co3O4 monolayer microsphere arrays uniformly cover the surface of the rGO/CNTs film. The alkaline hydrothermal treatment leads to not only the deposition of Co3O4 microspheres array, but also the reduction of the GO sheets at the same time. The unique hybrid paper is evaluated as an electrode for electrochemical capacitors without any ancillary materials. It is found that the obtained hybrid flexible paper, composed of Co3O4 microsphere array anchored to the underling conductive rGO/CNTs substrate with robust adhesion, is able to deliver high specific capacitance with excellent electrochemical stability even at high current densities, suggesting its promising application as an efficient electrode material for electrochemical capacitors.