Orthogonal-Channel, Low-Tortuosity Carbon Nanotube Platforms for High-Performance Li–O2 Batteries

Aerogels and foams are promising electrode materials owing to their lightweight, high porosity, and large surface area for creating abundant active/catalytic sites. Tailoring their porous structure is essential toward maximum electrode performance yet remains challenging in the field. Here, by modifying a pristine carbon nanotube (CNT) sponge with random internal distribution, we present a CNT platform consisting of regular, orthogonally intercrossed through-channels centered at a suitable lateral size (around 5 μm), with low tortuosity and enhanced electrochemical kinetics under predefined compression. Our CNT platforms, grafted by bifunctional transitional metal hydroxide catalyst, overcome considerable challenges of both long cycle life and high rates simultaneously, serving as Li-O2 cathodes and achieving lifetime of 500 cycles at 0.5 mA cm-2 (275 cycles even at 1 mA cm-2) and also displaying high areal capacity (27 mA h cm-2), which are superior to most of the recently reported porous electrodes based on various materials. The mechanism involving fast triple-phase transport and reversible discharge product deposition, enabled by catalyst-loaded orthogonal channels, has been disclosed. Such structure-tailored robust CNT platforms could find many applications in electrochemical catalysis and energy storage systems.