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<p>Redox-active porous aromatic frameworks (PAFs) have emerged as hopeful candidates for sodium-ion batteries (SIBs) in view of their porous structures, chemical stability and tunable architectures. Herein, we successfully synthesized two redox-active PAFs (PAF-305 and PAF-306) with different nitrogen-containing motifs, and demonstrated their application as cathode materials for SIBs. Density functional theory (DFT) calculations reveal that nitrogen-rich PAF-305 exhibits a lower lowest unoccupied molecular orbital (LUMO) energy level (−3.35 eV) and a narrower energy gap (<i>E</i><sub>g</sub>) (2.40 eV) compared with nitrogen-poor PAF-306. As expected, PAF-305 displays outstanding electrochemical performance, comprising a high reversible capacity of 145.2 mAh g<sup>−1</sup> at 0.05 A g<sup>−1</sup> and satisfactory cycling stability with 92% capacity retention over 1000 cycles at 0.2 A g<sup>−1</sup>. Remarkably, PAF-305 maintains robust electrochemical properties across a wide temperature range (−20 °C to 50 °C). Through a combination of experimental characterizations and theoretical calculations, the sodium-ion storage mechanism of PAF-305 is elucidated. This study not only provides a promising strategy for exploring other redox-active organic units in the design of novel PAFs, but also expands the potential applications of PAFs in energy storage systems.</p>

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Planting nitrogen-rich motif into porous aromatic frameworks to boost redox potential and multi-ion storage for wide-temperature sodium-organic batteries

  • 期刊论文

  • 发表日期：

    2025年10月27日

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  • Mimi Zhang,
  • Linqi Cheng,
  • Zhaoli Liu,
  • Fengchao Cui,
  • Fang Luo,
  • Heng-Guo Wang

摘要

Redox-active porous aromatic frameworks (PAFs) have emerged as hopeful candidates for sodium-ion batteries (SIBs) in view of their porous structures, chemical stability and tunable architectures. Herein, we successfully synthesized two redox-active PAFs (PAF-305 and PAF-306) with different nitrogen-containing motifs, and demonstrated their application as cathode materials for SIBs. Density functional theory (DFT) calculations reveal that nitrogen-rich PAF-305 exhibits a lower lowest unoccupied molecular orbital (LUMO) energy level (−3.35 eV) and a narrower energy gap (Eg) (2.40 eV) compared with nitrogen-poor PAF-306. As expected, PAF-305 displays outstanding electrochemical performance, comprising a high reversible capacity of 145.2 mAh g−1 at 0.05 A g−1 and satisfactory cycling stability with 92% capacity retention over 1000 cycles at 0.2 A g−1. Remarkably, PAF-305 maintains robust electrochemical properties across a wide temperature range (−20 °C to 50 °C). Through a combination of experimental characterizations and theoretical calculations, the sodium-ion storage mechanism of PAF-305 is elucidated. This study not only provides a promising strategy for exploring other redox-active organic units in the design of novel PAFs, but also expands the potential applications of PAFs in energy storage systems.