High-Coulombic-Efficiency Lithium Metal Anodes Enabled by Three-Dimensional Lithiophilic Nanostructures with Multiscale Porosity

The formation and growth of lithium dendrites have dramatically limited the application of lithium metal anodes due to their shortened lifespan and safety hazards. We fabricated a three-dimensional (3D) matrix comprised of interconnected NiO/Ni nanobranches linking carbon fibers in carbon cloth (NiO/Ni/CC). In-situ transformation of NiO to Li2O/Ni renders stronger binding between the carbon cloth and lithium ions, guiding homogeneous lithium plating in nano- and microscale pores of nanobranches. In parallel, the macroscale pores between carbon fibers in a 3D framework facilitate the infiltration of electrolytes and thus regulate ion transport. The NiO/Ni/CC showcases excellent electrochemical reversibility upon lithium plating/stripping with an exceptionally high Coulombic efficiency of 99.97% for 800 cycles, and an excellent cycling stability of 700 h at a a high current density of 3 mA cm–2 for a high areal capacity of 3 mAh cm–2. Moreover, full cells paired with both LiFePO4 and LiNi0.5Co0.2Mn0.3O2 cathodes demonstrate a superior rate capability and stability. This work manifests an efficient and scalable route on the dual design of lithiophilicity and porosity of 3D lithium metal hosts for high-performance lithium metal batteries