<p>An all-solid-state lithium–sulfur cell employing a lithium phosphorus sulfur chloride (Li<sub>6</sub>PS<sub>5</sub>Cl) solid-state electrolyte and electroless-tin-plated sulfur solid-state composite cathodes is demonstrated as a viable architecture for next-generation energy-storage systems. To investigate the role of tin-plating layer, tin-plated sulfur cathodes with systematically varied tin contents are synthesized and evaluated. Owing to the optimized electronic conduction network and enhanced sulfur redox kinetics, the tin-plated sulfur 25 (tin-plated sulfur composites containing 25 wt% tin) cathode exhibits improved rate performance, delivering high discharge capacities of 1502, 1247, 1046, and 620&#xa0;mA h g<sup>–1</sup> at C/10, C/2, 1&#xa0;C, and 2&#xa0;C rates, respectively. During long-term cycling at a C/2 rate, the all-solid-state cell with tin-plated sulfur 25 cathode achieves a high initial capacity of 1226&#xa0;mA h g<sup>–1</sup> and retains 80% of its capacity after 1000 cycles, indicating excellent cyclability. Moreover, stable operation is further maintained over 10,000 cycles at high 1&#xa0;C rate with a discharge/charge efficiency approaching 100%. Even under high sulfur loading, the tin-plated sulfur 25 cathode sustains an areal capacity of 4&#xa0;mA h cm<sup>–2</sup>. The enhanced electrochemical performance originates from the dual functionality of tin plating, which establishes continuous electron-transport pathways while simultaneously facilitating solid–solid sulfur redox reactions, in combination with the high ionic conductivity and interfacial compatibility of the Li<sub>6</sub>PS<sub>5</sub>Cl electrolyte. These results highlight the effectiveness of hybrid metal–sulfur composite cathodes integrated with sulfide solid electrolytes, providing a promising pathway toward safe, high-energy-density all-solid-state lithium–sulfur batteries.</p> Graphical abstract <p></p>

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Tin-plated sulfur composite cathodes enabled by solid-state sulfide electrolyte for durable high-rate all-solid-state lithium–sulfur cells

  • Shih-Lun Yang,
  • Chih-Long Tsai,
  • Rüdiger-A. Eichel,
  • Sheng-Heng Chung

摘要

An all-solid-state lithium–sulfur cell employing a lithium phosphorus sulfur chloride (Li6PS5Cl) solid-state electrolyte and electroless-tin-plated sulfur solid-state composite cathodes is demonstrated as a viable architecture for next-generation energy-storage systems. To investigate the role of tin-plating layer, tin-plated sulfur cathodes with systematically varied tin contents are synthesized and evaluated. Owing to the optimized electronic conduction network and enhanced sulfur redox kinetics, the tin-plated sulfur 25 (tin-plated sulfur composites containing 25 wt% tin) cathode exhibits improved rate performance, delivering high discharge capacities of 1502, 1247, 1046, and 620 mA h g–1 at C/10, C/2, 1 C, and 2 C rates, respectively. During long-term cycling at a C/2 rate, the all-solid-state cell with tin-plated sulfur 25 cathode achieves a high initial capacity of 1226 mA h g–1 and retains 80% of its capacity after 1000 cycles, indicating excellent cyclability. Moreover, stable operation is further maintained over 10,000 cycles at high 1 C rate with a discharge/charge efficiency approaching 100%. Even under high sulfur loading, the tin-plated sulfur 25 cathode sustains an areal capacity of 4 mA h cm–2. The enhanced electrochemical performance originates from the dual functionality of tin plating, which establishes continuous electron-transport pathways while simultaneously facilitating solid–solid sulfur redox reactions, in combination with the high ionic conductivity and interfacial compatibility of the Li6PS5Cl electrolyte. These results highlight the effectiveness of hybrid metal–sulfur composite cathodes integrated with sulfide solid electrolytes, providing a promising pathway toward safe, high-energy-density all-solid-state lithium–sulfur batteries.

Graphical abstract