Tailoring Lithium Horizontal Deposition for Long-Lasting High-Loading NCA (≥5 mA h cm)||Lithium-Metal Full Cells in Carbonate Electrolytes.

We report a design for a synergistic lithium (Li) metal hosting layer for high-loading Li(Ni,Co,Al)O (NCA) (≥5 mA h cm)||Li-metal full cells in carbonate electrolytes. Based on density functional theory calculations, the hosting layer was designed as a three-dimensional silver/carbon composite nanofiber (Ag/CNF) network with high Li affinity and a platinum (Pt)-coated polypropylene separator with low Li affinity. This design enabled the tailoring of horizontal Li deposition on the Ag/CNF hosting layer. The Li deposition behavior modulated by the hosting layer was thoroughly examined based on the initial Li deposition and cycling behaviors of the Li||Li symmetric cell configuration. Cryogenic focused-ion beam cross-sectional images of the cycled Li anodes clearly demonstrated that dense lithium deposition was enabled by the synergistic hosting layer high-loading NCA (≥5 mA h cm)||Li-metal full cells. When the hosting layer was used, the average cycling performance improved by 78.27% under various cycling conditions. Our work demonstrates that the synergistic hosting layer design is a fruitful pathway to accelerate the commercialization of high-energy-density Li-metal batteries in carbonate electrolytes.