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<p>Lithium dendrite formation poses a significant safety hazard in lithium-ion batteries (LIBs), severely impeding their widespread adoption and further technological advancements. Here, we present a novel quaternized polybenzimidazolium (<i>q</i>-PBI) to armor polyimide (PI) nanofiber separator (<i>q</i>-PBI@PI), in which the <i>q</i>-PBI containing lithiophilicity and anionphilicity sites serves as the multifunctional nano-layers to suppress the Li dendrite and reinforce the mechanical properties of PI nanofiber separator. Specifically, the <i>q</i>-PBI@PI separator displays an unprecedented mechanical strength of 82.8 MPa, significantly outperforming previously reported PI nanofiber membranes (typically below 50.0 MPa). Besides, we demonstrate that the <i>q</i>-PBI@PI separator simultaneously possesses low nucleation overpotential (59 mV) and exceptional average coulombic efficiency due to the suppression of Li dendrite. Importantly, <i>q</i>-PBI@PI-based Li∥Li battery enables a stable Li plating-stripping at 1.0 mA cm<sup>−2</sup> for 600 h. Attributing to these exceptional merits, the armored PI separator-based LIBs display remarkable specific capability and capacity retention. The density function theory calculations reveal that <i>q</i>-PBI is conducive to the desolvation of Li<sup>+</sup> and can immobilize Li<sup>+</sup> and PF<sub>6</sub><sup>−</sup> ions near affinity sites of PI nanofibers for inhibiting the formation of Li dendrites. Our work paves a new avenue for the design of next-generation high-performing separators in LIBs.</p>

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Polybenzimidazolium-reinforced polyimide separators to inhibit dendrites for high-security lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2025年1月3日

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  • Guohua Sun,
  • Jiaqi Cui,
  • Qingsong Zhang,
  • Yisong Zhou,
  • Xinluo Li,
  • Yingying Zhang,
  • Zhanao Zhang,
  • Xin Zhang,
  • Jiantao Fan,
  • Pengpeng Li,
  • Lianlong Hou,
  • Nanjun Chen

摘要

Lithium dendrite formation poses a significant safety hazard in lithium-ion batteries (LIBs), severely impeding their widespread adoption and further technological advancements. Here, we present a novel quaternized polybenzimidazolium (q-PBI) to armor polyimide (PI) nanofiber separator (q-PBI@PI), in which the q-PBI containing lithiophilicity and anionphilicity sites serves as the multifunctional nano-layers to suppress the Li dendrite and reinforce the mechanical properties of PI nanofiber separator. Specifically, the q-PBI@PI separator displays an unprecedented mechanical strength of 82.8 MPa, significantly outperforming previously reported PI nanofiber membranes (typically below 50.0 MPa). Besides, we demonstrate that the q-PBI@PI separator simultaneously possesses low nucleation overpotential (59 mV) and exceptional average coulombic efficiency due to the suppression of Li dendrite. Importantly, q-PBI@PI-based Li∥Li battery enables a stable Li plating-stripping at 1.0 mA cm−2 for 600 h. Attributing to these exceptional merits, the armored PI separator-based LIBs display remarkable specific capability and capacity retention. The density function theory calculations reveal that q-PBI is conducive to the desolvation of Li+ and can immobilize Li+ and PF6− ions near affinity sites of PI nanofibers for inhibiting the formation of Li dendrites. Our work paves a new avenue for the design of next-generation high-performing separators in LIBs.