Graphene Carbon Nanotube Carpets Grown Using Binary Catalysts for High-Performance Lithium-Ion Capacitors

Here we show that a versatile binary catalyst solution of Fe3O4/AlOx nanoparticles enables homogeneous growth of single to few-walled carbon nanotube (CNT) carpets from three-dimensional carbon-based substrates, moving past existing two-dimensional limited growth methods. The binary catalyst is composed of amorphous AlOx nanoclusters over Fe3O4 crystalline nanoparticles, facilitating the creation of seamless junctions between the CNTs and the underlying carbon platform. The resulting graphene-CNT (GCNT) structure is a high-density CNT carpet ohmically connected to the carbon substrate, an important feature for advanced carbon electronics. As a demonstration of the utility of this approach, we use GCNTs as anodes and cathodes in binder-free lithium-ion capacitors, producing stable devices with high-energy densities (∼120 Wh kg–1), high-power density capabilities (∼20,500 W kg–1 at 29 Wh kg–1), and a large operating voltage window (4.3 to 0.01 V).