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<p>The incessant quest for high-energy-density batteries to meet the growing demand of electrification makes high-level safety operation a critical concern. Traditional polypropylene separators, susceptible to thermal instability and sodium dendrite growth, often lead to internal short circuits and catastrophic thermal runaway. Here, a flame-retardant, dendrite-suppressing, and ion-regulating hydrogen-bonded organic framework (HOF) separator is designed by a simple and scalable strategy. The HOF lattice, featuring abundant polar N–H and C=O sites, preferentially coordinates PF<sub>6</sub><sup>−</sup>. This selective interaction suppresses anion migration, yielding a high Na<sup>+</sup> transference number (0.91). Concurrently, the liquid-filled pores and weakly coordinating channels of the HOF facilitate rapid Na<sup>+</sup> transport, achieving an ionic conductivity of 1.57&#xa0;mS&#xa0;cm<sup>−1</sup> at 60&#xa0;°C. Interfacial analyses reveal that the HOF stabilizes Na<sup>+</sup> deposition by fostering a NaF-rich solid electrolyte interphase with a high Young’s modulus (~ 11 GPa), which suppresses dendrite penetration. Furthermore, thermogravimetric and combustion tests confirm exceptional resilience above 380&#xa0;°C and the formation of carbon nitride layer that effectively suppresses heat release. Consequently, Na||Na symmetric cells cycle stably for over 2000 h at 2&#xa0;mA&#xa0;cm<sup>−2</sup>, while Na||Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> full cells retain high capacity ~ 99% over 5000 cycles at 5&#xa0;C. A pouch cell with a Prussian blue cathode further demonstrates practical applicability with consistent operation at 0.5&#xa0;C. This multifunctional HOF separator establishes a new paradigm for stable, fast, selective, dendrite-free, and fire-safe sodium metal batteries. </p>

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A Flame-Retardant Hydrogen-Bonded Organic Framework Separator for Selective Sodium-Ion Transport toward a NaF-Rich Interphase in Sodium Metal Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月9日

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  • Muhammad Ali,
  • Moazzam Ali,
  • Hamid Hussain,
  • Samia Aman,
  • Ufra Naseer,
  • Asif Mahmood,
  • Muhammad Tayyab Ahsan,
  • Yinzhu Jiang,
  • Muhammad Yousaf

摘要

The incessant quest for high-energy-density batteries to meet the growing demand of electrification makes high-level safety operation a critical concern. Traditional polypropylene separators, susceptible to thermal instability and sodium dendrite growth, often lead to internal short circuits and catastrophic thermal runaway. Here, a flame-retardant, dendrite-suppressing, and ion-regulating hydrogen-bonded organic framework (HOF) separator is designed by a simple and scalable strategy. The HOF lattice, featuring abundant polar N–H and C=O sites, preferentially coordinates PF6−. This selective interaction suppresses anion migration, yielding a high Na+ transference number (0.91). Concurrently, the liquid-filled pores and weakly coordinating channels of the HOF facilitate rapid Na+ transport, achieving an ionic conductivity of 1.57 mS cm−1 at 60 °C. Interfacial analyses reveal that the HOF stabilizes Na+ deposition by fostering a NaF-rich solid electrolyte interphase with a high Young’s modulus (~ 11 GPa), which suppresses dendrite penetration. Furthermore, thermogravimetric and combustion tests confirm exceptional resilience above 380 °C and the formation of carbon nitride layer that effectively suppresses heat release. Consequently, Na||Na symmetric cells cycle stably for over 2000 h at 2 mA cm−2, while Na||Na3V2(PO4)3 full cells retain high capacity ~ 99% over 5000 cycles at 5 C. A pouch cell with a Prussian blue cathode further demonstrates practical applicability with consistent operation at 0.5 C. This multifunctional HOF separator establishes a new paradigm for stable, fast, selective, dendrite-free, and fire-safe sodium metal batteries.