PNNL

Abstract

Spatial and morphology control over lithium (Li) metal nucleation/growth, as well as improving Li Coulombic efficiency (CE) are of the most challenging issues for rechargeable Li metal batteries. Here, we report that LiAsF6 and vinylene carbonate (VC) can work synergistically to address these challenges. It is revealed that AsF6- can be reduced to Li3As and LiF, which can act as seeds for Li growth and form a robust solid electrolyte interphase (SEI) layer, respectively. The addition of VC is critical because it not only enables uniform AsF6- reduction by passivating the defect sites on Cu substrate, but also improves the SEI layer flexibility during the reductive polymerization process. As a result, highly compact, uniform and dendrite-free Li film with vertically aligned columns structure can be obtained with greatly increased Li CE, and the Li metal batteries using the electrolyte with both LiAsF6 and VC additives can have much improved cycle life.