Anode Overpotential Control via Interfacial Modification: Inhibition of Lithium Plating on Graphite Anodes.

Lithium-metal deposition on graphite anodes limits the cycle life and negatively impacts safety of the current state of the art Li-ion batteries. Herein, deliberate interfacial modification of graphite electrodes via direct current (DC) magnetron sputtering of nanoscale layers of Cu and Ni is employed to increase the overpotential for Li deposition and suppress Li plating under high rate charge conditions. Due to their nanoscale, the deposited surface films have minimal impact (∼0.16% decrease) on cell level theoretical energy density. Interfacial properties of the anodes are thoroughly characterized by atomic force microscopy (AFM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and spatially resolved mapping X-ray absorption near edge structure (XANES) spectroscopy. The spectroscopic measurements indicate that the Cu and Ni coatings form oxide upon exposure to an ambient environment, but they are reduced within the electrochemical cell and remain in a metallic state. Li plating is quantified by X-ray diffraction and associated electrochemistry measurements revealing that the surface treatment effectively reduces the quantity of the plated Li metal by ∼50% compared to untreated electrodes. These results establish an effective method using interfacial modification to achieve deliberate control of Li-metal deposition overpotential and reduction of lithium plating on graphite.