Electrochemically induced crystalline-to-amorphization transformation in sodium samarium silicate solid electrolyte for long-lasting sodium metal batteries

Ge Sun, Chenjie Lou, Boqian Yi, Wanqing Jia, Zhixuan Wei, Shiyu Yao (), Ziheng Lu (), Gang Chen, Zexiang Shen, Mingxue Tang () and Fei Du ()
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Ge Sun: Jilin University
Chenjie Lou: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Boqian Yi: Jilin University
Wanqing Jia: Jilin University
Zhixuan Wei: Jilin University
Shiyu Yao: Jilin University
Ziheng Lu: University of Cambridge
Gang Chen: Jilin University
Zexiang Shen: Jilin University
Mingxue Tang: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Fei Du: Jilin University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Exploiting solid electrolyte (SE) materials with high ionic conductivity, good interfacial compatibility, and conformal contact with electrodes is essential for solid-state sodium metal batteries (SSBs). Here we report a crystalline Na5SmSi4O12 SE which features high room-temperature ionic conductivity of 2.9 × 10−3 S cm−1 and a low activation energy of 0.15 eV. All-solid-state symmetric cell with Na5SmSi4O12 delivers excellent cycling life over 800 h at 0.15 mA h cm−2 and a high critical current density of 1.4 mA cm−2. Such excellent electrochemical performance is attributed to an electrochemically induced in-situ crystalline-to-amorphous (CTA) transformation propagating from the interface to the bulk during repeated deposition and stripping of sodium, which leads to faster ionic transport and superior interfacial properties. Impressively, the Na|Na5SmSi4O12|Na3V2(PO4)3 sodium metal batteries achieve a remarkable cycling performance over 4000 cycles (6 months) with no capacity loss. These results not only identify Na5SmSi4O12 as a promising SE but also emphasize the potential of the CTA transition as a promising mechanism towards long-lasting SSBs.

Date: 2023
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DOI: 10.1038/s41467-023-42308-0

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