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/AlO_x 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 AlO_x 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).