Flexible Graphene/Carbon Nanotube Electrochemical Double-Layer Capacitors with Ultrahigh Areal Performance

The fabrication of electrochemical double-layer capacitors (EDLCs) with high areal capacitance relies on the use of elevated mass loadings of highly porous active materials. Herein, we demonstrate a high-throughput manufacturing of graphene/carbon nanotubes hybrid EDLCs. The wet-jet milling (WJM) method is exploited to exfoliate the graphite into single-few-layer graphene flakes (WJM-G) in industrial volumes (production rate ca. 0.5 kg/day). Commercial single-/double-walled carbon nanotubes (SDWCNTs) are mixed with graphene flakes in order to act as spacers between the flakes during their film formation. The WJM-G/SDWCNTs films are obtained by one-step vacuum filtration of the material dispersions, resulting in self-standing, metal- and binder-free flexible EDLC electrodes with high active material mass loadings up to around 30 mg cm^-2 . The corresponding symmetric WJM-G/SDWCNTs EDLCs exhibit electrode energy densities of 539 μWh cm^-2 at 1.3 mW cm^-2 and operating power densities up to 532 mW cm^-2 (outperforming most of the reported EDLC technologies). The EDCLs show excellent cycling stability and outstanding flexibility even in highly folded states (up to 180°).