Lithiophilic current collector based on nitrogen doped carbon nanotubes and three-dimensional graphene for long-life lithium metal batteries

• Porous 3DG decorated with NCNT is employed as effective hosts for lithium metal. • NCNT-3DG host material with enhanced lithiophilicity and reduced volume variation. • Long lifespan at high current density of Li metal electrode can be realized. • The Li@NCNT-3DG electrodes ensure an enhanced performance of Li-S full cells. Lithium metal as an attractive anode material has been widely used in advanced energy storage devices. However, drawbacks such as growth of lithium dendrites, significant volume changes during the cycling process, causing safety hazards and limited span-life, have impeded the commercial application of lithium metal anode. Here, we present a new composite structure, consisting of porous three-dimensional graphene (3DG) decorated with nitrogen-doped carbon nanotubes (NCNT). The created NCNT-3DG carbon scaffold is resilient towards significant volumetric change during cycling, while the NCNTs serve as lithiophilic sites for uniform lithium nucleation which enables uniform lithium deposition. This novel hybrid endows the lithium anode with a long-term stability reaching up to 1200 cycles at high current density of 10 mA cm −2 . This significantly improved the performance of the created lithium-sulfur full cells. The demonstrated performance of the NCNT-3DG structure provides new insights for the designing and fabrication of metallic lithium anodes.