Synthesis of Interconnected Graphene Framework with Two-Dimensional Protective Layers for Stable Lithium Metal Anodes

Severe lithium (Li) dendrite growth during the plating/stripping process, which results in low Coulombic efficiency and safety issues, strongly hinders the practical applications of Li metal anodes. Herein, we propose a novel design of three-dimensional (3D) interconnected graphene (IG) framework synthesized with the help of nickel (Ni) microspheres for stable Li metal anodes. The as-prepared IG framework consists of multiple stacks of two-dimensional (2D) graphene layers and plenty of hollow graphene microspheres in between, and thus provides protective layers on the top to suppress lithium dendrites, sufficient surface area to reduce the effective current density, as well as ion channels for fast Li transport, which is confirmed by post-cycle morphology characterization. When Li foil was used as the counter electrode for Li deposition, the assembled coin cell maintained an average Coulombic efficiency of more than 97.5% for 100 cycles at current density of 1 mA cm−2 with a Li loading of 1 mAh cm−2. Furthermore, we achieved stable cycling for more than 300 h at a current density of 1 mA cm−2 with a Li loading of 2 mAh cm−2 when assembled as symmetric cells. This strategy of vertically stacking 2D materials provides a novel approach towards dendrite-free Li metal anodes for the next-generation energy storage systems.