Mirror-Like Electrodeposition of Lithium Metal under a Low-Resistance Artificial Solid Electrolyte Interphase Layer

Nonuniform electrodeposition and dendritic growth of lithium metal coupled to its chemical incompatibility with liquid electrolytes are largely responsible for poor Coulombic efficiency and safety hazards preventing the successful implementation of energy-dense Li metal anodes. Artificial solid electrolyte interface (ASEI) layers have been proposed to address the morphological evolution and chemical reactions in Li metal anodes. In this study, an ASEI layer consisting of a lithium phosphorus oxynitride (LiPON) thin film electrolyte and gold-alloying interlayer was developed and shown to promote the electrodeposition of smooth, homogeneous, mirror-like Li metal morphologies. The Au layer alloyed with Li, reducing the nucleation overpotential and resulting in a more spatially uniform metal deposit, while the LiPON layer provided a physical barrier between the Li metal and aprotic liquid electrolyte. The effectiveness and integrity of the LiPON protective layer was assessed using in operando impedance spectroscopy and ex situ SEM/EDS characterization. Smooth, homogeneous Li morphologies were realized in capacities up to 3 mAh cm^-2 plated at 0.1 mA cm^-2. At higher current densities up to 1 mA cm^-2 or increased deposition capacities of 6 mAh cm^-2, the LiPON coating fractured due to the localized, nonuniform lithium deposits and rough, dendritic Li morphologies were observed. This approach represents a new strategy in the design of artificial SEIs to enable Li metal anodes with practical areal capacities.