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<p>2D covalent organic frameworks (COFs) usually possess a polycrystalline nature as well as lower porosity and surface area than 3D counterparts, restraining their exploration over gas storage applications. Herein, a substituent strategy has been proposed and employed to generate three robust single-crystal 2D COFs isomers with atom-resolution structures determined by 3D electron diffraction. Among three isomers, a precise engineering of their interlayer distance affords the highest Brunauer−Emmett−Teller surface area of ~2100 m<sup>2</sup> g<sup>−1</sup> and the largest pore volume of 1.40 cm<sup>3</sup> g<sup>−1</sup> for the desolvated GZU-1. This COF shows the highest total volumetric methane uptake of 240 cm<sup>3</sup> (STP) cm<sup>−3</sup> at 273 K and 100 bar among 2D COFs, even comparable with those for excellent 3D MOFs. This work not only delivers unique insight into the design of 2D single-crystal COFs by interlayer stacking regulation, but also promotes the application of highly porous 2D COFs in gas storage.</p>

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Single-crystal 2D covalent organic frameworks for high-capacity methane storage

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月14日

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  • Baoqiu Yu,
  • Felipe L. Oliveira,
  • Wenliang Li,
  • Qingmei Xu,
  • Xu Ding,
  • Shangwei Yuan,
  • Yucheng Jin,
  • Hua Liu,
  • Hailong Wang,
  • Xin Xiao,
  • Jingping Zhang,
  • Guillaume Maurin,
  • Banglin Chen,
  • Jianzhuang Jiang

摘要

2D covalent organic frameworks (COFs) usually possess a polycrystalline nature as well as lower porosity and surface area than 3D counterparts, restraining their exploration over gas storage applications. Herein, a substituent strategy has been proposed and employed to generate three robust single-crystal 2D COFs isomers with atom-resolution structures determined by 3D electron diffraction. Among three isomers, a precise engineering of their interlayer distance affords the highest Brunauer−Emmett−Teller surface area of ~2100 m2 g−1 and the largest pore volume of 1.40 cm3 g−1 for the desolvated GZU-1. This COF shows the highest total volumetric methane uptake of 240 cm3 (STP) cm−3 at 273 K and 100 bar among 2D COFs, even comparable with those for excellent 3D MOFs. This work not only delivers unique insight into the design of 2D single-crystal COFs by interlayer stacking regulation, but also promotes the application of highly porous 2D COFs in gas storage.