Correlating the Microstructure and Current Density of the Li/Garnet Interface.

Abstract

Solid-state lithium batteries hold great promise for next-generation energy storage systems. However, the formation of lithium filaments within the solid electrolyte remains a critical challenge. In this study, we investigate the crucial role of morphology in determining the resistance of garnet-type electrolytes to lithium filaments. By proposing a new test method, namely, cyclic linear sweep voltammetry, we can effectively evaluate the electrolyte resistance against lithium filaments. Our findings reveal a strong correlation between the microscopic morphology of the solid electrolyte and its resistance to lithium filaments. Samples with reduced pores and multiple grain boundaries demonstrate remarkable performance, achieving a critical current density of up to 3.2 mA cm-2 and excellent long-term cycling stability. Kelvin probe force microscopy and finite element method simulation results shed light on the impact of grain boundaries and electrolyte pores on lithium-ion transport and filament propagation. To inhibit lithium penetration, minimizing pores and achieving a uniform morphology with small grains and plenty of grain boundaries are essential.