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<p>Covalently bonded crystalline substances with micropores have broad applications. Covalent organic frameworks (COFs) are representative of such substances. They have so far been classified into two-dimensional (2D) and three-dimensional (3D) COFs. 2D-COFs have planar shapes useful for broad purposes, but obtaining good crystals of 2D-COFs with sizes larger than 10 μm is significantly challenging, whereas yielding 3D-COFs with high crystallinity and larger sizes is easier. Here, we show COFs with 2.5-dimensional (2.5D) skeletons, which are microscopically constructed with 3D bonds but have macroscopically 2D planar shapes. The 2.5D-COFs shown herein achieve large single-crystal sizes above 0.1 mm and ultrahigh-density primary amines regularly allocated on and pointing perpendicular to the covalently-bonded network plane. Owing to the latter nature, the COFs are promising as CO<sub>2</sub> adsorbents that can simultaneously achieve high CO<sub>2</sub>/N<sub>2</sub> selectivity and low heat of adsorption, which are usually in a mutually exclusive relationship. 2.5D-COFs are expected to broaden the frontier and application of covalently bonded microporous crystalline systems.</p>

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2.5-dimensional covalent organic frameworks

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月2日

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  • Tomoki Kitano,
  • Syunto Goto,
  • Xiaohan Wang,
  • Takayuki Kamihara,
  • Yoshihisa Sei,
  • Yukihito Kondo,
  • Takumi Sannomiya,
  • Hidehiro Uekusa,
  • Yoichi Murakami

摘要

Covalently bonded crystalline substances with micropores have broad applications. Covalent organic frameworks (COFs) are representative of such substances. They have so far been classified into two-dimensional (2D) and three-dimensional (3D) COFs. 2D-COFs have planar shapes useful for broad purposes, but obtaining good crystals of 2D-COFs with sizes larger than 10 μm is significantly challenging, whereas yielding 3D-COFs with high crystallinity and larger sizes is easier. Here, we show COFs with 2.5-dimensional (2.5D) skeletons, which are microscopically constructed with 3D bonds but have macroscopically 2D planar shapes. The 2.5D-COFs shown herein achieve large single-crystal sizes above 0.1 mm and ultrahigh-density primary amines regularly allocated on and pointing perpendicular to the covalently-bonded network plane. Owing to the latter nature, the COFs are promising as CO2 adsorbents that can simultaneously achieve high CO2/N2 selectivity and low heat of adsorption, which are usually in a mutually exclusive relationship. 2.5D-COFs are expected to broaden the frontier and application of covalently bonded microporous crystalline systems.