Robust Expandable Carbon Nanotube Scaffold for Ultrahigh‐Capacity Lithium‐Metal Anodes

Abstract There has been a renewed interest in using lithium (Li) metal as an anode material for rechargeable batteries owing to its high theoretical capacity of 3860 mA h g −1 . Despite extensive research, modifications to effectively inhibit Li dendrite growth still result in decreased Li loading and Li utilization. As a result, real capacities are often lower than values expected, if the total mass of the electrode is taken into consideration. Herein, a lightweight yet mechanically robust carbon nanotube (CNT) paper is demonstrated as a freestanding framework to accommodate Li metal with a Li mass fraction of 80.7 wt%. The highly conductive network made of sp2‐hybridized carbon effectively inhibits formation of Li dendrites and affords a favorable coulombic efficiency of >97.5%. Moreover, the Li/CNT electrode retains practical areal and gravimetric capacities of 10 mA h cm −2 and 2830 mA h g −1 (vs the mass of electrode), respectively, with 90.9% Li utilization for 1000 cycles at a current density of 10 mA cm −2 . It is demonstrated that the robust and expandable nature is a distinguishing feature of the CNT paper as compared to other 3D scaffolds, and is a key factor that leads to the improved electrochemical performance of the Li/CNT anodes.