A Freestanding 3D Skeleton with Gradationally Distributed Lithiophilic Sites for Realizing Stable Lithium Anodes

Lithium (Li) metal anodes are drawing considerable attention owing to their ultrahigh theoretical capacities and low electrochemical reduction potentials. However, their commercialization has been hampered by safety hazards induced by continuous dendrite growth. These issues can be alleviated using the ZnO-modified 3D carbon-based host containing carbon nanotubes (CNTs) and carbon felt (CF) fabricated by electroplating in the present study (denoted as ZnO/CNT@CF). The constructed skeleton has lithiophilic ZnO that is gradationally distributed along its thickness. The utilization of an inverted ZnO/CNT@CF-Li anode obtained by flipping over the carbon skeleton after Li electrodeposition is also reported herein. The synergistic effect of the Li metal and lithiophilic sites reduces the nucleation overpotential, thus inducing Li⁺ to preferentially deposit inside the porous carbon-based scaffold. The composite electrode compels Li to grow away from the separator, thereby significantly improving battery safety. A symmetric cell with the inverted ZnO/CNT@CF-Li electrode operates steadily for 700 cycles at 1 mA cm^-2 and 1 mAh cm^-2 . Moreover, the ZnO/CNT@CF-Li|S cell exhibits an initial areal capacity of 10.9 mAh cm^-2 at a S loading of 10.4 mg cm^-2 and maintains a capacity of 3.0 mAh cm^-2 after 320 cycles.