Guided Lithium Metal Deposition and Improved Lithium Coulombic Efficiency through Synergistic Effects of LiAsF₆ and Cyclic Carbonate Additives

Spatial and morphology control over lithium (Li) metal nucleation and growth, as well as improving Li Coulombic efficiency (CE), are among the most challenging issues for rechargeable Li metal batteries. Here, we report that LiAsF₆ and cyclic carbonate additives such as vinylene carbonate (VC) or fluoroethylene carbonate (FEC) can work synergistically to address these challenges. It is revealed that LiAsF₆ can be reduced to Li_xAs alloy and LiF, which act as nanosized seeds for Li growth and form a robust solid electrolyte interface layer. The addition of VC or FEC not only enables the uniform distribution of Li_xAs seeds but also improves the flexibility of the solid electrolyte interface layer. As a result, highly compact, uniform, and dendrite-free Li film with vertically aligned column structure can be obtained with increased Li CE, and the Li metal batteries using the electrolyte with both LiAsF₆ and cyclic carbonate additives can have improved cycle life.