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<p>Radicals arranged in a two-dimensional (2D) hexagonal network can offer various exotic magnetic, electronic, and optical properties that find application in electronics/spintronics. However, direct synthesis remains challenging due to the scarcity of stable, symmetry-matched radical building blocks. Here, we report the bottom-up synthesis of hexagonal 2D radical covalent organic frameworks (RCOFs) with unpaired electrons at the nodes of the frameworks. A planar verdazyl radical amine (V-NH<sub>2</sub>) undergoes Schiff-base condensation with aldehydes to afford highly crystalline hexagonal RCOFs (VTPT and VPMT). The spin density was precisely controlled through the selection of building blocks with modulated spin-spin distances. The EPR and SQUID measurements confirmed a high spin concentration with antiferromagnetic interactions at low temperature, which is further tuned by interlayer interactions. Thin films of VTPT exhibited preferential in-plane orientation with enhanced photoconductivity, attributed to improved π-conjugation. These findings establish a direct route to RCOFs and underscore their potential as pseudo 1-dimensional antiferromagnetic materials.</p>

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Direct Construction of Magnetic and Electrical Two-Dimensional Radical Covalent Organic Frameworks

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月23日

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  • Rajendra Prasad Paitandi,
  • Madhurima Giri,
  • Ryosuke Koyae,
  • Masaki Nobuoka,
  • Yusuke Tsutsui,
  • Yoshiaki Shuku,
  • Yun Hee Koo,
  • Zhuowei Li,
  • Yuta Sakurai,
  • Katsuaki Suzuki,
  • Javier López-Cabrelles,
  • Shuhei Furukawa,
  • Hironori Kaji,
  • Masayuki Suda,
  • Samrat Ghosh,
  • Shu Seki

摘要

Radicals arranged in a two-dimensional (2D) hexagonal network can offer various exotic magnetic, electronic, and optical properties that find application in electronics/spintronics. However, direct synthesis remains challenging due to the scarcity of stable, symmetry-matched radical building blocks. Here, we report the bottom-up synthesis of hexagonal 2D radical covalent organic frameworks (RCOFs) with unpaired electrons at the nodes of the frameworks. A planar verdazyl radical amine (V-NH2) undergoes Schiff-base condensation with aldehydes to afford highly crystalline hexagonal RCOFs (VTPT and VPMT). The spin density was precisely controlled through the selection of building blocks with modulated spin-spin distances. The EPR and SQUID measurements confirmed a high spin concentration with antiferromagnetic interactions at low temperature, which is further tuned by interlayer interactions. Thin films of VTPT exhibited preferential in-plane orientation with enhanced photoconductivity, attributed to improved π-conjugation. These findings establish a direct route to RCOFs and underscore their potential as pseudo 1-dimensional antiferromagnetic materials.