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

Erik A. Wu, Swastika Banerjee, Hanmei Tang, Peter M. Richardson, Jean-Marie Doux, Ji Qi, Zhuoying Zhu, Antonin Grenier, Yixuan Li, Enyue Zhao, Grayson Deysher, Elias Sebti, Han Nguyen, Ryan Stephens, Guy Verbist, Karena W. Chapman, Raphaële J. Clément (), Abhik Banerjee (), Ying Shirley Meng () and Shyue Ping Ong ()
Additional contact information
Erik A. Wu: University of California San Diego
Swastika Banerjee: University of California San Diego
Hanmei Tang: University of California San Diego
Peter M. Richardson: University of California Santa Barbara
Jean-Marie Doux: University of California San Diego
Ji Qi: University of California San Diego
Zhuoying Zhu: University of California San Diego
Antonin Grenier: Stony Brook University
Yixuan Li: University of California San Diego
Enyue Zhao: University of California San Diego
Grayson Deysher: University of California San Diego
Elias Sebti: University of California Santa Barbara
Han Nguyen: University of California San Diego
Ryan Stephens: Shell International Exploration & Production Inc.
Guy Verbist: Shell Global Solutions International BV
Karena W. Chapman: Stony Brook University
Raphaële J. Clément: University of California Santa Barbara
Abhik Banerjee: University of California San Diego
Ying Shirley Meng: University of California San Diego
Shyue Ping Ong: University of California San Diego

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-21488-7

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