A Lightweight, Adhesive, Dual-Functionalized Over-Coating Interphase Toward Ultra-Stable High-Current Density Lithium Metal Anodes

Coherent manipulation of the lithium plating pattern is at the heart of the safe operation of metallic anodes in the battery technologies. In this article, a lightweight (~0.3 mg cm⁻²), dual-functionalized carbon spheres are anchored onto the Cu foil as the interfacial protective layer via the chelation process of the catechol groups in the polydopamine precursor and the copper foil. The dual-functionalized carbon spheres exhibit the intriguing complementary features: Lithiophilic nitrogen dopants favor the Li⁺ ion absorption and mitigate the nucleation barrier, while the micro/mesopore reservoir spatially homogenizes the ion flux distribution, confining the metallic propagation without dendrite-like protrusions. The metallic anode exhibits an ultra-stable plating/stripping process for 1400 hr with the average Coulombic efficiency of ~99%. A full-cell prototype is constructed by pairing the N-doped carbon spheres on the bare Cu (NCS-Cu) electrode with the high-mass-loading LiVPO₄F (12.5 mg cm⁻²) cathode that can deliver a high energy density of 421.2 Wh kg⁻¹ with the highest power density of 2106 W kg⁻¹ to promise the anode use for high-power/energy-dense metallic batteries.