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<p>Three-dimensional (3D) covalent organic frameworks (COFs) hold significant promise for a variety of applications. However, conventional design approaches using regular building blocks limit the structural diversity of 3D COFs. Here we design and synthesize two 3D COFs, designated as JUC-644 and JUC-645, through a methodology that relies on using eight-connected building blocks with reduced symmetry. Their structures are solved using continuous rotation electron diffraction and high-resolution transmission electron microscopy, which reveal a unique linkage with a double chain structure, a rare phenomenon in COFs. We deconstruct these structures into [4 + 3(+ 2)]-c nets, which leads to six different topologies. Furthermore, JUC-644 demonstrates high adsorption capacity for C<sub>3</sub>H<sub>8</sub> and <i>n</i>-C<sub>4</sub>H<sub>10</sub> (11.28 and 10.45 mmol g<sup>−1</sup> at 298 K and 1 bar, respectively), surpassing most known porous materials, with notable selectivity for C<sub>3</sub>H<sub>8</sub>/C<sub>2</sub>H<sub>6</sub> and <i>n</i>-C<sub>4</sub>H<sub>10</sub>/C<sub>2</sub>H<sub>6</sub>. This approach opens avenues for designing intricate architectures and shows the potential of COFs in C<sub>2</sub>H<sub>6</sub> recovery from natural gas liquids.</p><p></p>

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Synthesis of three-dimensional covalent organic frameworks through a symmetry reduction strategy

  • 期刊论文

  • 发表日期：

    2025年1月8日

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  • Jianhong Chang,
  • Zeyue Zhang,
  • Haorui Zheng,
  • Hui Li,
  • Jinquan Suo,
  • Chunqing Ji,
  • Fenqian Chen,
  • Shipeng Zhang,
  • Zitao Wang,
  • Valentin Valtchev,
  • Shilun Qiu,
  • Junliang Sun,
  • Qianrong Fang

摘要

Three-dimensional (3D) covalent organic frameworks (COFs) hold significant promise for a variety of applications. However, conventional design approaches using regular building blocks limit the structural diversity of 3D COFs. Here we design and synthesize two 3D COFs, designated as JUC-644 and JUC-645, through a methodology that relies on using eight-connected building blocks with reduced symmetry. Their structures are solved using continuous rotation electron diffraction and high-resolution transmission electron microscopy, which reveal a unique linkage with a double chain structure, a rare phenomenon in COFs. We deconstruct these structures into [4 + 3(+ 2)]-c nets, which leads to six different topologies. Furthermore, JUC-644 demonstrates high adsorption capacity for C3H8 and n-C4H10 (11.28 and 10.45 mmol g−1 at 298 K and 1 bar, respectively), surpassing most known porous materials, with notable selectivity for C3H8/C2H6 and n-C4H10/C2H6. This approach opens avenues for designing intricate architectures and shows the potential of COFs in C2H6 recovery from natural gas liquids.