Sustainable Release of LiNO3 from a Fluorine-Decorated Metal-Organic Framework Separator to Enable High-Performance Li-Metal Batteries in Carbonate Electrolytes

MC Du and ZB He and YQ Zhang and YP Cai and QF Zheng, ADVANCED ENERGY MATERIALS, 15, 2403674 (2025).

DOI: 10.1002/aenm.202403674

High-voltage Li-metal batteries hold great prospects for boosting energy density, while the Li-metal anodes show poor compatibility with high- voltage tolerant carbonate electrolytes, leading to unstable solid- electrolyte interphase (SEI) and uncontrolled Li dendrites growth. Herein, a F-decorated UIO-66/polyimide (PI) functional separator encapsulated with LiNO3 (LNO@UIO-66F/PI) is rationally designed to regulate the interfacial chemistry and Li deposition behavior. Specifically, the UIO-66F nanoparticles in situ grown on the PI fibers form continuous electronegative nanochannels, which promote rapid and uniform Li+ flux while repelling the anion migration. Furthermore, the LiNO3 encapsulated in the UIO-66F nanopores sustainably releases to form a thin and conductive Li3N-rich SEI. This synergy effect induces a dense and spherical Li deposition behavior, effectively inhibiting the growth of Li dendrites. Consequently, this LNO@UIO-66F/PI separator demonstrates highly reversible Li plating/stripping over 1000 h at an extremely high current density of 10 mA cm(-2) in carbonate electrolytes, and also enables the stable cycling of Li||LiNi0.8Co0.1Mn0.1O2 cell over 1000 cycles under a high cut-off voltage of 4.5 V, paving the way for practical application of high- energy-density Li-metal batteries.

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