Rechargeable Metal-Sulfur Batteries: Key Materials to Mechanisms.

Rechargeable metal-sulfur batteries are considered promising candidates for energy storage due to their high energy density along with high natural abundance and low cost of raw materials. However, they could not yet be practically implemented due to several key challenges: (i) poor conductivity of sulfur and the discharge product metal sulfide, causing sluggish redox kinetics, (ii) polysulfide shuttling, and (iii) parasitic side reactions between the electrolyte and the metal anode. To overcome these obstacles, numerous strategies have been explored, including modifications to the cathode, anode, electrolyte, and binder. In this review, the fundamental principles and challenges of metal-sulfur batteries are first discussed. Second, the latest research on metal-sulfur batteries is presented and discussed, covering their material design, synthesis methods, and electrochemical performances. Third, emerging advanced characterization techniques that reveal the working mechanisms of metal-sulfur batteries are highlighted. Finally, the possible future research directions for the practical applications of metal-sulfur batteries are discussed. This comprehensive review aims to provide experimental strategies and theoretical guidance for designing and understanding the intricacies of metal-sulfur batteries; thus, it can illuminate promising pathways for progressing high-energy-density metal-sulfur battery systems.

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

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.

Highly Efficient Organosulfur and Lithium-Metal Hosts Enabled by C@Fe3 N Sponge.

Lithium-organosulfur (Li-OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li-OS batteries under realistic conditions. A well-designed freestanding carbon sponge decorated with Fe3 N nanoparticles (C@Fe3 N) is introduced into the Li-OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe3 N leads to an extremely stable cycling performance over 1 000 cycles in a Li-OS full cell under realistic conditions.

Anode-Free Lithium-Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules.

The two major barriers of practical lithium-sulfur batteries are the poor reversibility of lithium-metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. We show that SnI4 coordinates with lithium polysulfides to form soluble complexes, resulting in a Li2 SnS3 -rich anode interphase layer. As Li2 SnS3 is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI4 and lithium polysulfides play a non-negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode-free, lean-electrolyte pouch cells with a Li2 S cathode that displays capacity retention of 78 % after 100 cycles.