Unveiling the role of lithiophilic sites denseness in regulating lithium ion deposition

An insight into the effect of lithiophilic sites denseness on determining the Li ion depositing behaviors was proposed. The construction of lithiophilic sites is an effective way to achieve uniform lithium (Li) ion deposition for stably cycling Li metal batteries. However, in-depth investigations involving lithiophilic sites denseness (LSD) in impacting Li ion deposition remain unknown. Herein we propose an insight into this issue by probing the effect of LSD on determining the Li ion deposition. Experimental characterization and theoretical simulation demonstrate that rational LSD plays a vital role in both Li nucleation and the subsequent Li ion plating behaviors. By tailoring the LSD from low to high, the accompanied Li nucleation overpotentials continuously decrease. Additionally, the Li ion mobility increases first and then weakens in the subsequent Li ion plating stage. Consequently, the Li metal with a moderate LSD allows a dendrite-free morphology and satisfactory long-term cycling performances. This work affords a deeper fundamental understanding of lithiophilic chemistry that directs the development of efficient strategies to realize dendrite-free Li metal batteries.