Zirconia-free NaSICON Solid Electrolyte Materials for Sodium All-solid-state Batteries

Tieu, A. J. K.; Mahayoni, E.; Li, Y.; Deng, Z.; Fauth, F.; Chotard, J.-N.; Seznec, V.; Adams, S.; Masquelier, C.; Canepa, P.

doi:10.1039/D3TA04665F

Zirconia-free NaSICON Solid Electrolyte Materials for Sodium All-solid-state Batteries

A. J. K. Tieu, E. Mahayoni, Y. Li, Z. Deng, F. Fauth, J.-N. Chotard, V. Seznec, S. Adams, C. Masquelier, and P. Canepa; J. Mater. Chem. A 11, 23233 (2023).

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BibTeX

@article{Tieu2023zirconia,
  author  = {Tieu, A. J. K. and Mahayoni, E. and Li, Y. and Deng, Z. and Fauth, F. and Chotard, J.-N. and Seznec, V. and Adams, S. and Masquelier, C. and Canepa, P.},
  title   = {{Zirconia-free NaSICON Solid Electrolyte Materials for Sodium All-solid-state Batteries}},
  journal = {Journal of Materials Chemistry A},
  volume  = {11},
  pages   = {23233},
  year    = {2023},
  doi     = {10.1039/D3TA04665F}
}

Brief summary

The NaSICON solid electrolyte Na_1+xZr₂Si_xP_3−xO₁₂ almost always contains zirconia as an impurity, which can lower its conductivity. By adjusting the amount of zirconium in the synthesis, we make it free of zirconia, and it reaches a total sodium conductivity of about 3.5 mS cm⁻¹ at room temperature, an excellent conductor for all-solid-state sodium batteries.

Full abstract

The growing demand for energy storage systems sparks a race to build inexpensive and safer rechargeable batteries. All-solid-state sodium (Na)-ion batteries are a competitive alternative to their lithium (Li) analogs due to the lower cost of Na resources. The Na SuperIonic CONductors Na_1+xZr₂Si_xP_3-xO₁₂ 0 ≤ x ≤ 3 (NZSP) are widely studied as solid electrolytes. However, synthesized NZSPs always contain m-ZrO₂ as the main impurity phase, which may lead to a lower Na-ion ionic conductivity within the solid-electrolyte layer. Here, we synthesize zirconia-free NZSP by engineering the quantity of Zirconium (Zr) precursors. Synchrotron X-Ray diffraction, Raman spectroscopy, and density functional theory simulations reveal zirconia-free NZSP. Impedance spectroscopy measurement of zirconia-free NZSP reveals an impressive total ionic conductivity of ~3.49 mS cm⁻¹ with a bulk conductivity of ~10.05 mS cm⁻¹ at room temperature, making it an excellent Na-ion conductor for all-solid-state batteries. These results pave the way towards the synthesis optimization of impurity-free complex solid-electrolytes, which are important if solid-state batteries are to be commercialized.