Dendrite Growth Suppression in Lithium Metal Batteries with Composite Quasi-solid Electrolytes

Abstract

Secondary batteries are crucial for eco-friendly systems, but existing technologies struggle with energy density and safety issues. This study aims to develop a next-generation battery utilizing quasi-solid electrolytes (QSE), which combine the advantages of both liquid and solid electrolytes. However, QSEs often lack the mechanical strength necessary to prevent lithium dendrite growth. To address this challenge, two strategies were proposed and experimentally validated. The first strategy involves creating a QSE-separator composite (QSE-PI) by integrating QSE with a polyimide (PI) separator. Among the various options, PI with a thickness greater than 20 μm and a pore size of 2-5 μm exhibited superior electrolyte absorption and dendrite suppression. This configuration allowed for rapid lithium plating/stripping, high ionic conductivity (1.7 × 10-3 S cm-1), and excellent Coulombic efficiency (99.94%).The second strategy incorporates silica (SiO2) as a ceramic filler in the QSE-PI to enhance mechanical strength and ion transport. The addition of SiO2 disrupted polymer crystallinity, increased the amorphous regions, and effectively suppressed dendrite formation. Notably, SiO2 particles larger than 10 μm improved cycle stability, with the composite maintaining performance for over 50 cycles, compared to only 30 cycles for the version without filler.