Monolithic All-Solid-State High-Voltage Li-Metal Thin-Film Rechargeable Battery

Abstract

The substitution of an organic liquid electrolyte with lithium-conducting solid materials is a promising approach to overcome the limitations associated with conventional lithium-ion batteries. These constraints include a reduced electrochemical stability window, high toxicity, flammability, and the formation of lithium dendrites. In this way, all-solid-state batteries present themselves as ideal candidates for improving energy density, environmental friendliness, and safety. In particular, all-solid-state configurations allow the introduction of compact, lightweight, high-energy-density batteries, suitable for low-power applications, known as thin-film batteries. Moreover, solid electrolytes typically offer wide electrochemical stability windows, enabling the integration of high-voltage cathodes and permitting the fabrication of higher-energy-density batteries. A high-voltage, all-solid-state lithium-ion thin-film battery composed of LiNi0.5Mn1.5O4 cathode, a LiPON solid electrolyte, and a lithium metal anode has been deposited layer by layer on low-cost stainless-steel current collector substrates. The structural and electrochemical properties of each electroactive component of the battery had been analyzed separately prior to the full cell implementation. In addition to a study of the internal solid–solid interface, comparing them was done with two similar cells assembled using conventional lithium foil, one with thin-film solid electrolyte and another one with thin-film solid electrolyte plus a droplet of LP30 liquid electrolyte. The thin-film all-solid state cell developed in this work delivered 80.5 mAh g–1 in the first cycle at C/20 and after a C-rate test of 25 cycles at C/10, C/5, C/2, and 1C and stabilized its capacity at around 70 mAh g–1 for another 12 cycles prior to the start of its degradation. This cell reached gravimetric and volumetric energy densities of 333 Wh kg–1 and 1,212 Wh l–1, respectively. Overall, this cell showed a better performance than its counterparts assembled with Li foil, highlighting the importance of the battery interface control.