Layer-opened graphene paper with carbon nanotubes as support in a flexible electrode material for supercapacitors

Graphene paper is a promising electrode material for use in flexible supercapacitors due to its good electronic conductivity and excellent mechanical characteristics. However, layers of graphene paper have a strong tendency to restack, resulting in a seriously reduced specific surface area and limited electrochemical performance. In this paper, restacked layers of graphene paper are reopened by a vacuum-assisted method, and carbon nanotubes (CNTs) are directly deposited on the enlarged space between the opened graphene layers. Consequently, an ordered carbon composite structure with alternately arranged graphene sheets and CNTs is constructed and exhibits increased specific surface area and a 3D conductive network. The structure and morphology of the samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy and N2 adsorption/desorption measurements. The electrochemical performance was tested by galvanostatic charge-discharge test (GDC), electrochemical impedance spectroscopy (EIS) and cyclic voltammograms (CV). The obtained graphene/CNT paper exhibits a remarkably improved capacity of 170.8 F g−1, which is nearly two times higher than that obtained for a regular graphene paper.