DOI: 10.1021/acs.nanolett.6c03756 ISSN: 1530-6984

Engineering a Dynamic Alloy–Fluoride Interface via a Co-Placement Gas-Phase Strategy for Stable Lithium Metal Anodes

Siyi Hu, Saisai Li, Jiawen Xiao, Changbo Yu, Ning Li, Jidong Cao, Hao Luo, Dawei Zhang

Abstract

Lithium metal batteries (LMBs) hold great promise for next-generation high-energy-density energy storage systems, but suffer from uneven Li nucleation and unstable interfaces. Here, a scalable coplacement gas-phase reaction strategy is developed to construct an adaptive alloy–fluoride interface on nickel mesh current collectors, enabling one-step in-situ formation of a uniform Ni3Sb/NiF2 layer. The lithiophilic Ni3Sb alloy effectively lowers the lithium nucleation barrier and guides uniform lithium deposition. Upon cycling, NiF2 is transformed into a LiF-rich interphase, which stabilizes the electrode/electrolyte interface and homogenizes Li+ flux. The combined interface enables durable and uniform Li plating/stripping under long-term cycling. Consequently, the Ni3Sb/NiF2-modified anode achieves stable cycling for over 2600 h in symmetric cells and delivers 83.1% capacity retention after 240 cycles in LiFePO4 full cells with a high areal capacity of 10 mAh cm–2. This work provides a facile and scalable strategy for engineering multifunctional interfaces toward practical LMBs.

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