Publication date: 10th April 2024
All-solid-state sodium batteries have been attracting attentions owing to their safety and abundant raw material resources. The suitable solid electrolyte is a key factor to enable the commercialization of all-solid-state batteries. Chloride solid electrolytes have attracted attention due to high ionic conductivity, oxidation stability, and room temperature processability. Fewer sodium-ion conducting chlorides have been developed compared to lithium-ion conducting materials. It is necessary to discover the chlorides as the end-member of sodium-ion conductors. We recently reported the development of a new NaTaCl6 chloride as an end-member sodium-ion conductor [1]. Although NaTaCl6 has high oxidation stability, its conductivity and reduction stability are still low, and further increases are needed.
Herein, we report the oxyhalides in the pseudo-ternary system NaCl–TaCl5–Ta2O5 (hereinafter denoted to Na1+5xTaCl6–5xO5x (x = 0.05, 0.1, 0.15, 0.2, 0.25, and 0.3) with high conductivity, formability, and oxidation and reduction stabilities. The mechanochemically prepared samples were composed of NaCl and Ta2O5 nanoparticles embedded in the Na–Ta–Cl–O amorphous matrix. The Na2.25TaCl4.75O1.25 samples showed the ionic conductivity of 2.5×10–3 S cm–1 at 25 ºC and the electrochemical potential window of 0.4 – 4.1 vs. Na+/Na. We have succeeded in developing the solid electrolyte balanced with conductivity and electrochemical stability.
This work was partly supported by JSPS KAKENHI (Grant Numbers: JP21H04701 and JP19H05816), MEXT Program: Data Creation and Utilization-Type Material Research and Development Project Grant Number JPMXP1122712807, and JST Adopting Sustainable Partnerships for Innovative Research Ecosystem Grant Number JPMJAP2313.
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