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Integrated high-sulfur-loading polysulfide/carbon cathode in lean-electrolyte cell toward high-energy-density lithium–sulfur cells with stable cyclability
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2023-03-27 , DOI: 10.1039/d3ta00210a
Yun-Chen Wu, Sheng-Heng Chung

The commercialization of high-energy-density lithium–sulfur batteries depends on the development of a high-sulfur-loading cathode with high electrochemical utilization and stability in lean-electrolyte cells. However, the desired cell-design parameters often exacerbate the sluggish conversion reaction between sulfur and sulfide and intensify polysulfide diffusion. This results in low specific capacity, considerable capacity degradation, and a short cycle life, thus worsening the electrochemical performance. Here, we present a new design of the cathode material and configuration: a core–shell polysulfide/carbon cathode. The cathode contains a high amount of high-activity polysulfide catholyte as its active core, and the catholyte is sealed in a conductive shell made of an entangled fabric-like, tubular carbon tissue with low nanoporosity. The material design allows for fast redox kinetics and charge transfer, and the designed cell configuration stabilizes the electrochemical reaction. Thus, the lean-electrolyte lithium–sulfur cell achieves a record low electrolyte-to-sulfur ratio (4–3 μL mg−1), while enabling the core–shell polysulfide/carbon cathode with a high sulfur loading and content (12 mg cm−2 and 64.1 wt%, respectively) to exhibit a high peak charge-storage capacity (832 mA h g−1 at a 0.10C rate), high rate performance (0.10C–0.20C), and long-term cyclability with high capacity retention approaching 70% after 200 cycles.

中文翻译:

贫电解质电池中的集成高载硫多硫化物/碳阴极可实现具有稳定循环性能的高能量密度锂硫电池

高能量密度锂硫电池的商业化取决于在贫电解质电池中具有高电化学利用率和稳定性的高载硫正极的开发。然而,所需的电池设计参数通常会加剧硫和硫化物之间缓慢的转化反应,并加剧多硫化物的扩散。这会导致比容量低、容量显着下降和循环寿命短,从而恶化电化学性能。在这里,我们提出了一种新的阴极材料和配置设计:核壳多硫化物/碳阴极。阴极包含大量高活性多硫化物阴极电解液作为其活性核心,阴极电解液密封在由缠结的织物状管状碳组织制成的导电壳中,具有低纳米孔隙率。材料设计允许快速氧化还原动力学和电荷转移,并且设计的电池配置稳定了电化学反应。因此,贫电解质锂硫电池实现了创纪录的低电解质硫比(4-3 μL mg−1 ),同时使具有高硫负载和含量(分别为 12 mg cm −2和 64.1 wt%)的核壳多硫化物/碳阴极表现出高峰值电荷存储容量(832 mA hg −1在0.10C倍率)、高倍率性能(0.10C-0.20C)和长期循环性能,200次循环后容量保持率接近70%。
更新日期:2023-03-31
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