Honeycomb Inspired Lithiophilic Scaffold for Ultra-Stable, High-Areal-Capacity Metallic Deposition

The uncontrolled nucleation behavior and the “hostless” Li propagation seriously hinder the commercialization of metallic Li anodes in the next-generation energy-dense batteries. Here we propose a honeycomb-inspired, high-strength scaffold with the tunable microstructural features to accommodate the Li deposits via a “pore-filling” behavior. The complementary components in the Al-Al_xO_y-C composite comprise the alloy-induced Li-Al intermediate embryos for the preferential nucleation and mixed-conducting nanosheet scaffold to homogenize the ion/electron mass transfer; as a result, the in-plane mechanical stress is accommodated during the substantial metal loading. This composite scaffold delivers a sustained Li plating/stripping cycling for 1700 h and exhibits high-areal-capacity value up to 15 mA h cm⁻² with the stable Coulombic efficiency over 99.5%. In the as-constructed full-cell (2 mA h) which integrates the Al-Al_xO_y-C metallic anode and the LiNi_0.8Mn_0.1Co_0.1O₂ cathode, the impressive energy densities of 454.4 Wh kg⁻¹ and robust cyclability up to 300 cycles are realized. The alloy-induced metallic deposition process, validated by the operando X-ray diffraction and density functional theory calculations, illustrates the competitive lithiation mechanism within the honeycomb scaffold.