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<p>Polyethylene oxide (PEO)-based solid polymer electrolytes are considered as promising material for solid-state sodium metallic batteries (SSMBs). However, their poor interfacial stability with high-voltage cathode limits their application in high-energy–density solid-state batteries. Herein, a uniform, sulfur-containing inorganic–organic composite cathode–electrolyte interphase layer was in situ formed by the addition of sodium polyvinyl sulfonate (NaPVS). The 5&#xa0;wt% NaPVS-Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (NVP)|PEO-sodium hexauorophosphate (NaPF<sub>6</sub>)|Na battery shows a higher initial capacity of 111.2&#xa0;mAh·g<sup>−1</sup> and an ultra-high capacity retention of 90.5% after 300 cycles. The 5&#xa0;wt% NaPVS-Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>2</sub>F<sub>3</sub> (NVPF) |PEO-NaPF<sub>6</sub>|Na battery with the high cutoff voltage of 4.2&#xa0;V showed a specific discharge capacity of 88.9&#xa0;mAh·g<sup>−1</sup> at 0.5C for 100 cycles with a capacity retention of 79%, which is much better than that of the&#xa0;pristine-NVPF (PR-NVPF)|PEO-NaPF<sub>6</sub>|Na battery (33.2%). The addition of NaPVS not only enhances the diffusion kinetics at the interface but also improves the rate performance and stability of the battery, thus bolstering its viability for high-energy applications. In situ phase tracking further elucidates that NaPVS effectively mitigates self-discharge induced by the oxidative decomposition of PEO at high temperature. This work proposes a general strategy to maintain the structural stability of the cathode–electrolyte interface in PEO-based high-performance SSMBs.</p> Graphical abstract <p></p>

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Multifunctional sulfonate additive induced CEI layer enables ultra-stable PEO based solid-state sodium batteries

  • 期刊论文

  • 发表日期：

    2025年3月5日

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  • Jing-Chao Liu,
  • Tao You,
  • Yi-Fan Zhao,
  • Feng-Quan Liu,
  • Jie-Dong Li,
  • Long-Long Wang,
  • Chen Wang,
  • Lin Li

摘要

Polyethylene oxide (PEO)-based solid polymer electrolytes are considered as promising material for solid-state sodium metallic batteries (SSMBs). However, their poor interfacial stability with high-voltage cathode limits their application in high-energy–density solid-state batteries. Herein, a uniform, sulfur-containing inorganic–organic composite cathode–electrolyte interphase layer was in situ formed by the addition of sodium polyvinyl sulfonate (NaPVS). The 5 wt% NaPVS-Na3V2(PO4)3 (NVP)|PEO-sodium hexauorophosphate (NaPF6)|Na battery shows a higher initial capacity of 111.2 mAh·g−1 and an ultra-high capacity retention of 90.5% after 300 cycles. The 5 wt% NaPVS-Na3V2(PO4)2F3 (NVPF) |PEO-NaPF6|Na battery with the high cutoff voltage of 4.2 V showed a specific discharge capacity of 88.9 mAh·g−1 at 0.5C for 100 cycles with a capacity retention of 79%, which is much better than that of the pristine-NVPF (PR-NVPF)|PEO-NaPF6|Na battery (33.2%). The addition of NaPVS not only enhances the diffusion kinetics at the interface but also improves the rate performance and stability of the battery, thus bolstering its viability for high-energy applications. In situ phase tracking further elucidates that NaPVS effectively mitigates self-discharge induced by the oxidative decomposition of PEO at high temperature. This work proposes a general strategy to maintain the structural stability of the cathode–electrolyte interface in PEO-based high-performance SSMBs.

Graphical abstract