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| Home > Publications database > Na+-ion conducting ceramics with superior performances |
| Conference Presentation (Invited) | FZJ-2026-01359 |
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2025
Abstract: The huge demand for delocalized energy storage due to the application of fluctuating energy sources leads to a need for low-cost devices available on a large scale and with high energy density. Sodium-based batteries show great potential in this field and have recently attracted extensive interest. Solid electrolytes (SEs) rather than liquid electrolytes display the advantages of non-leakage, non-volatilization, adaptability to temperature changes as well as compatible theoretical energy and power densities, which makes solid-state sodium batteries (SSNBs) potentially the batteries of the next generation. Plenty of Na-ion conducting SEs have been reported until now, such like ceramics, sulfides, boranes, chlorides, glasses, polymers, etc.1 In this presentation, ceramics are specially addressed because of their high stability in normal atmosphere and low cost. Ceramics are defined as crystalline, non-metallic, inorganic materials which are usually formed by the application of sintering. Presently most of the reported ion conducting ceramics are oxides, including NaSICONs, Na5LnSi4O12 (Ln = La-Lu and Y), beta-alumina, Na2X2TeO6 (X = transition metal), Na2O-TiO2 based ceramics, etc.1 The development of the former two types is a particular focus at our institute due to their excellent performance and relative ease of handling. In the family of NaSICONs, Na3.4Zr2Si2.4P0.6O12 (NZSP) ceramics are reported with unaverage total conductivity (σtotal) of 5 × 10-3 S cm-1 at 25 °C.1-3 A remarkable Na dendrite-growth behavior along the ceramic surface rather than through the ceramic is also found for NZSP. Operando investigations and in situ SEM microelectrode experiments are conducted to reveal the Na plating mechanism. By covering the ceramic surface with sodium salt coatings, surface dendrite formation is prevented and the dendrite tolerance of Na | NZSP | Na symmetric cells is increased to a critical current density (CCD) of 14 mA cm−2 and galvanostatic cycling of 1 mA cm−2 / 1 mAh cm−2 (half cycle) is demonstrated for more than 1000 h.4 It should be further noticed that compared to the extraordinary bulk conductivity (σbulk, 15mS cm-2 at 25 °C), the σtotal of NZSP is only fair due to micro-crack formation caused by the thermal expansion anisotropy. We further modify the grain boundaries of NZSP by adding 1-5 mol% Na3LaP2O8 (NLP) or LaNbO4 (LNO) to counteract the micro-crack formation. The σtotal of NZSP-NLP and NZSP-LNO is increased to 7.1 and 9.3 mS cm−1 at 25 °C, respectively.5,6 The dendrite tolerance of the modified NZSP is also increased to the CCD of 22 mA cm-2 and galvanostatic cycling at 10 mA cm−2. For the cathode side, the inter-ceramic contact problems have also been solved by combining the infiltration of a porous electrolyte scaffold with precursor solution and in situ synthesis of electrode active material.3,7 The resulting cells using Na3V2P3O12 (NVP), NZSP and Na as the positive electrode, electrolyte and negative electrode materials, respectively, can be stably operated with a capacity of 0.55 mAh cm-2 at high rate of 0.5 mA cm-2. In addition, Na5LnSi4O12-type ceramic solidi electrolytes are also investigated because of their promising ionic conductivity similar to NaSICONs. Na5YSi4O12 (NYS) and Na4.92Y0.92Zr0.08Si4O12 (NYZS) show σtotal of 1.0 mS cm-1 and 3.3 mS cm-1 at 25 °C,8,9 respectively. The CCD of NYZS against Na metal electrodes can reach 2.4 mA cm-2.9 The galvanostatic cycling time is more than 1000 h applying 1 mA cm-2 and 1 mAh cm-2.9 With positive sulfur composite electrode, a Na/NYS/S pouch cell can be operated with specific capacity of about 600 mAh g-1 for more than 100 cycles.101. Q. Ma, F. Tietz, ChemElectroChem 2020, 7, 2693–2713; 2. Q. Ma et al., J. Mater. Chem. A, 2019, 7, 7766–7776; 3. C.-L. Tsai et al., J. Power Sources. 2020, 476, 228666; 4. Q. Ma et al., Adv. Energy Mater., 2022, 12, 2201680; 5. L. Liu et al., J. Power Sources 2025, 626, 235773; 6. L. Liu et al. Adv. Energy Mater. 2024, 14, 2404985; 7. T. Lan et al. Nano Energy, 2019, 65, 104040; 8. A. Yang et al., Chem. Eng. J., 2022, 435, 134774; 9. A. Yang et al., eScience 2023,3,100175; 10. A. Yang et al., Carbon Energy, 2023, 5, e371.
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