Directing (110) Oriented Lithium Deposition through High-flux Solid Electrolyte Interphase for Dendrite-free Lithium Metal Batteries

Controlling lithium (Li) electrocrystallization with preferred orientation is a promising strategy to realize highly reversible Li metal batteries (LMBs) but lack of facile regulation methods. Herein, we report a high-flux solid electrolyte interphase (SEI) strategy to direct (110) preferred Li deposition even on (200)-orientated Li substrate. Bravais rule and Curie-Wulff principle are expanded in Li electrocrystallization process to decouple the relationship between SEI engineering and preferred crystal orientation. Multi-spectroscopic techniques combined with dynamics analysis reveal that the high-flux CF3Si(CH3)3 (F3) induced SEI (F3-SEI) with high LiF and -Si(CH3)3 contents can ingeniously accelerate Li+ transport dynamics and ensure the sufficient Li+ concentration below SEI to direct Li (110) orientation. The induced Li (110) can in turn further promote the surface migration of Li atoms to avoid tip aggregation, resulting in a planar, dendrite-free morphology of Li. As a result, our F3-SEI enables ultra-long stability of Li||Li symmetrical cells for more than 336 days. Furthermore, F3-SEI modified Li can significantly enhance the cycle life of Li||LiFePO4 and Li||NCM811 coin and pouch full cells in practical conditions. Our crystallographic strategy for Li dendrite suppression paves a path to achieve reliable LMBs and may provide guidance for the preferred orientation of other metal crystals. (110) orientated lithium (Li) deposition is achieved via high-flux solid electrolyte interphase. Bravais rule and Curie-Wulff principle clarify Li electrocrystallization process. Long-term Li deposition regulation ability is realized. Planar and dendrite-free (110) orientated Li enables Li||LiFePO4, Li||NCM811 cells in practical conditions dramatically improved electrochemical performance.+image

Automated summary

A high-flux solid electrolyte interphase (SEI) strategy is used to achieve (110) orientated lithium deposition, even on (200)-orientated Li substrate. The SEI induced by CF3Si(CH3)3 promotes Li+ transport dynamics and directs Li (110) orientation. This method enables long-term stability and improved electrochemical performance of lithium metal batteries.