N-doped Porous Host with Lithiophilic Co Nanoparticles Implanted into 3D Carbon Nanotubes for Dendrite-Free Lithium Metal Anodes

Lithium (Li) metal is a promising anode material due to its high theoretical capacity (3860 mA h g–1) and lowest electrochemical potential. Nevertheless, the uncontrollable growth of Li dendrites and the infinite volume change during cycling restrict the practical applications of lithium metal batteries (LMBs). Herein, a dandelion-like host material, which is composed of a N-doped porous core with lithiophilic Co nanoparticles implanted into 3D carbon nanotubes (defined as Co@NPC), is developed to enable dendrite-free hybrid lithium metal anodes (HLMAs) even at high current density. The porous N-doped carbon polyhedron core inserted by lithiophilic Co nanoparticles provides high specific surface area and enriched nucleation sites to guide smooth lithium nucleation and deposition in the core with decreased nucleation barrier. Simultaneously, the nanochannel confinement effect of 3D carbon nanotubes inhibits the growth of dendrites and induces Li deposition into the internal space homogeneously. In virtue of the unique nanoarchitecture construction, the HLMA delivers superior Coulombic efficiency (98.3%) at a high current density of 5 mA cm–2 and exhibits ultralong lifespan (1000 cycles) with ultralow hysteresis voltage (31 mV) even at 10 mA cm–2. This work sheds light on designing and developing an advanced and scalable host for LMAs toward stable LMBs to be practical and feasible.