Lithiophilic 3D VN@N-rGO as a Multifunctional Interlayer for Dendrite-Free and Ultrastable Lithium-Metal Batteries.

It is still a big challenge to effectively suppress dendrite growth, which increases the safety and life of lithium-metal-based high energy/power density batteries. To address such issues, herein we design and fabricate a lithiophilic VN@N-rGO as a multifunctional layer on commercial polypropylene (PP) separator, which is constructed by a thin N-rGO nanosheet-wrapped VN nanosphere with a uniform pore distribution, relatively high lithium ionic conductivity, excellent electrolyte wettability, additional lithium-ion diffusion pathways, high mechanical strength, and reliable thermal stability, which are beneficial to regulate the interfacial lithium ionic flux, resulting in the formation of a stable and homogeneous current density distribution on Li-metal electrodes and hard modified separators that can resist dendrites piercing. Consequently, the growth of Li dendrite is effectively suppressed, and the cycle stability of lithium-metal batteries is significantly improved. In addition, even at a high current density of 10 mA cm and cutoff areal capacity of 5 mAh cm, the Li|Li symmetric batteries with VN@N-rGO/PP separators still work very well even over 2500 h, exhibiting ultrahigh cycling stability. This work presents rational design ideas and a facile fabrication strategy of a lithiophilic 3D porous multifunctional interlayer for dendrite-free and ultrastable lithium-metal-based batteries.