High-Loading Lithium-Sulfur Batteries with Solvent-Free Dry-Electrode Processing.

Abstract

Lithium-sulfur (Li-S) batteries, with their high energy density, nontoxicity, and the natural abundance of sulfur, hold immense potential as the next-generation energy storage technology. To maximize the actual energy density of the Li-S batteries for practical applications, it is crucial to escalate the areal capacity of the sulfur cathode by fabricating an electrode with high sulfur loading. Herein, ultra-high sulfur loading (up to 12 mg cm^-2) cathodes are fabricated through an industrially viable and sustainable solvent-free dry-processing method that utilizes a polytetrafluoroethylene binder fibrillation. Due to its low porosity cathode architecture formed by the binder fibrillation process, the dry-processed electrodes exhibit a relatively lower initial capacity compared to the slurry-processed electrode. However, its mechanical stability is well maintained throughout the cycling without the formation of electrode cracking, demonstrating significantly superior cycling stability. Additionally, through the optimization of the dry-processing, a single-layer pouch cell with a loading of 9 mg cm^-2 and a novel multi-layer pouch cell that uses an aluminum mesh as its current collector with a total loading of 14 mg cm^-2 are introduced. To address the reduced initial capacity of dry-processed electrodes, strategies such as incorporating electrocatalysts or employing prelithiated active materials are suggested.