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<p><i>sp</i><sup>2</sup>-carbon-linked covalent organic frameworks (<i>sp</i><sup>2</sup>c-COFs) are crystalline porous polymers with repeat organic units linked by <i>sp</i><sup>2</sup> carbons, and have attracted increasing interest due to their robust skeleton and tunable semiconducting properties. Single-crystalline <i>sp</i><sup>2</sup>c-COFs with well-defined structures can represent an ideal platform for investigating fundamental physics properties and device performance. However, the robust olefin bonds inhibit the reversible-reaction-based crystal self-correction, thus yielding polycrystalline or amorphous polymers. Here we report an imine-to-olefin transformation strategy to form single-crystal <i>sp</i><sup>2</sup>c-COFs. The isolated single crystals display rectangular nanotube-like domains with sizes up to approximately 24 μm × 0.8 μm × 0.8 μm, and permanent pore distribution around 1.1 nm. The highly conjugated olefin linkage endows the crystals with enhanced electronic connectivity which determines a remarkable room-temperature metal-free ferromagnetism (8.6 × 10<sup>−3</sup> emu g<sup>−1</sup>). Our protocol is robust and generally applicable for the synthesis of single-crystalline <i>sp</i><sup>2</sup>c-COFs for future spin-electron devices.</p><p></p>

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Synthesis of single-crystalline sp2-carbon-linked covalent organic frameworks through imine-to-olefin transformation

  • 期刊论文

  • 发表日期：

    2025年1月6日

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  • Shengxu Li,
  • Shunqi Xu,
  • En Lin,
  • Tonghai Wang,
  • Haoyong Yang,
  • Junyi Han,
  • Yuxiang Zhao,
  • Qunji Xue,
  • Paolo Samorì,
  • Zhenjie Zhang,
  • Tao Zhang

摘要

sp2-carbon-linked covalent organic frameworks (sp2c-COFs) are crystalline porous polymers with repeat organic units linked by sp2 carbons, and have attracted increasing interest due to their robust skeleton and tunable semiconducting properties. Single-crystalline sp2c-COFs with well-defined structures can represent an ideal platform for investigating fundamental physics properties and device performance. However, the robust olefin bonds inhibit the reversible-reaction-based crystal self-correction, thus yielding polycrystalline or amorphous polymers. Here we report an imine-to-olefin transformation strategy to form single-crystal sp2c-COFs. The isolated single crystals display rectangular nanotube-like domains with sizes up to approximately 24 μm × 0.8 μm × 0.8 μm, and permanent pore distribution around 1.1 nm. The highly conjugated olefin linkage endows the crystals with enhanced electronic connectivity which determines a remarkable room-temperature metal-free ferromagnetism (8.6 × 10−3 emu g−1). Our protocol is robust and generally applicable for the synthesis of single-crystalline sp2c-COFs for future spin-electron devices.