Threading the MOF-derived mesoporous carbon host with CNT network: An effective modification layer for high-areal-capacity Li metal anodes

The ramified lithium dendrite growth and severe volume expansion upon the metallic plating process impede the practical deployment of the lithium metal anode in the energy-dense battery system. In this article, a thin modification layer of the Al-based metal–organic framework (MOF) is carbonized into the mesoporous carbon nanorods (PCRs) with atomically dispersed lithiophilic sites; meanwhile these storage units are structurally reinforced by the in-situ grown carbon nanotubes. The interfacial engineered substrate (Al-PCRs/CNTs-Cu) exhibits an enhanced Li affinity with mitigated nucleation barrier, and thus realizes the long-lifespan up to 1000 h at high-capacity-loading of 8 mAh cm⁻². When integrating the modified substrate with LiN_0.8Co_0.1Mn_0.1O₂ (NCM-811) (∼10.5 mg cm⁻²) the cathode in a prelithiated full cell model (2*Li excess), the prototype exhibits a high energy density of 414.38 Wh kg⁻¹ at the highest power density of 1243.14 W kg⁻¹. This dual-functionalized, carbonaceous interfacial layer provides a facile and effective approach to construct the energy/power-dense metallic batteries.