Ni-embedding dendritic porous nanochannels promote internal lithium housing for dendrite-free lithium metal anodes

Architectural design of lithium metal anodes (LMAs) is crucial for smooth Li plating/stripping with suppressed dendrites, which is paramount for high-performance lithium metal batteries (LMBs). In this study, to leverage the carbonaceous host with low gravimetric density for enhanced Li accommodation and reversible Li deposition, mesoporous carbon nanocages comprising dendritic nanochannels embedded with lithophilic Ni nanoparticles are fabricated and exploited to mitigate superficial Li deposition and promote fast and reversible Li plating/stripping within the three-dimensional (3D) host of LMA. Through guided Li⁺ infiltration, enhanced Li⁺ diffusivity, lowered nucleation barrier, and expedited redox kinetics, the optimal Li host exhibits a high Coulombic efficiency of Li plating/stripping in Li-Cu half cells with significantly reduced dendrite formation and superb cycling stability of symmetric cells over 2000 h at 1 mA·cm⁻². When paired with the LiFePO₄ cathode, the LMB full cell demonstrates a prolonged cycle life, retaining 82.2% of its initial capacity after 600 cycles. This work highlights the crafting of 3D Li hosts with desired structure and functionality for guiding and accommodating smooth Li deposition.