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A stable cathode-solid electrolyte composite for high-voltage, long-cycle-life solid-state sodium-ion batteries.

  • Author(s): Wu, Erik A
  • Banerjee, Swastika
  • Tang, Hanmei
  • Richardson, Peter M
  • Doux, Jean-Marie
  • Qi, Ji
  • Zhu, Zhuoying
  • Grenier, Antonin
  • Li, Yixuan
  • Zhao, Enyue
  • Deysher, Grayson
  • Sebti, Elias
  • Nguyen, Han
  • Stephens, Ryan
  • Verbist, Guy
  • Chapman, Karena W
  • Clément, Raphaële J
  • Banerjee, Abhik
  • Meng, Ying Shirley
  • Ong, Shyue Ping
  • et al.
Abstract

Rechargeable solid-state sodium-ion batteries (SSSBs) hold great promise for safer and more energy-dense energy storage. However, the poor electrochemical stability between current sulfide-based solid electrolytes and high-voltage oxide cathodes has limited their long-term cycling performance and practicality. Here, we report the discovery of the ion conductor Na3-xY1-xZrxCl6 (NYZC) that is both electrochemically stable (up to 3.8 V vs. Na/Na+) and chemically compatible with oxide cathodes. Its high ionic conductivity of 6.6 × 10-5 S cm-1 at ambient temperature, several orders of magnitude higher than oxide coatings, is attributed to abundant Na vacancies and cooperative MCl6 rotation, resulting in an extremely low interfacial impedance. A SSSB comprising a NaCrO2 + NYZC composite cathode, Na3PS4 electrolyte, and Na-Sn anode exhibits an exceptional first-cycle Coulombic efficiency of 97.1% at room temperature and can cycle over 1000 cycles with 89.3% capacity retention at 40 °C. These findings highlight the immense potential of halides for SSSB applications.

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