N, F-enriched inorganic/organic composite interphases to stabilize lithium metal anodes for long-life anode-free cells.

ABSTRACT

The practical application of lithium metal batteries is considered to be one of the most promising successors for lithium-ion batteries due to their ability to meet the high-energy storage demands of modern society. However, their application is still hindered by the unstable solid electrolyte interphase (SEI) and uncontrollable dendrite growth. In this study, we propose a robust composite SEI (C-SEI) that consists of a fluorine doped boron nitride (F-BN) inner layer and an organic polyvinyl alcohol (PVA) outer layer. Both theoretical calculations and experimental results demonstrate that the F-BN inner layer induces the formation of favourable components (LiF and Li3N) at the interface, promoting rapid ionic transport and inhibiting electrolyte decomposition. The PVA outer layer acts as a flexible buffer in the C-SEI, ensuring the structural integrity of the inorganic inner layer during lithium plating and stripping. The C-SEI modified lithium anode shows a dendrite-free performance and stable cycle over 1200 h, with an ultralow overpotential (15 mV) at 1 mA cm-2 in this study. This novel approach also enhances the stability of capacity retention rate by 62.3% after 100 cycles even in anode-free full cells (C-SEI@Cu||LFP). Our findings suggest a feasible strategy for addressing the instability inherent in SEI, showing great prospects for the practical application of lithium metal batteries.