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<p>Multi-porous reticular materials, featuring various pore sizes and shapes, have gained increasing attention due to their structural properties that facilitate mass transport. However, the rational design of such materials remains challenging, particularly when selectively modulating pore sizes. Here we present a synthesis strategy that enables selective pore modulation in dual-porous layered double-walled hydrogen-bonded organic frameworks using triskele-shaped building units. We uncovered an unusual <i>syn</i> conformation of acylhydrazone, which forms hydrogen bonding with carboxyl groups, thereby allowing the rapid, scalable synthesis of a series of single crystals with exceptional stability, including resistance to aqua regia. Harnessing the enriched proton-hopping sites and acid robustness of the double-walled framework, we demonstrate that incorporating superacids into these dual-porous crystals effectively enhances proton conductivity, which reaches 4.25 × 10<sup>−3</sup> S cm<sup>−1</sup> at 30 °C. Furthermore, we elucidate the formation mechanism of double-walled hydrogen-bonded organic frameworks via a combination of experimental and computational approaches. This work opens avenues for the tailored design of multi-porous materials with independently tunable pore architectures and functionalities.</p><p></p>

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Selective pore modulation in layered molecular crystals

  • 期刊论文

  • 发表日期：

    2026年7月27日

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  • Qiang Gao,
  • Guoxing Jiang,
  • Xiang Liu,
  • Mingzi Sun,
  • Cheng Qian,
  • Chuting Yuan,
  • Walter P. D. Wong,
  • Jing Niu,
  • Yipu Xu,
  • Shutao Xu,
  • Guijun Ma,
  • Ziyi Li,
  • Jia-Wei Hu,
  • Peiyu Zhang,
  • Bolong Huang,
  • Wei Wei,
  • Xing Li

摘要

Multi-porous reticular materials, featuring various pore sizes and shapes, have gained increasing attention due to their structural properties that facilitate mass transport. However, the rational design of such materials remains challenging, particularly when selectively modulating pore sizes. Here we present a synthesis strategy that enables selective pore modulation in dual-porous layered double-walled hydrogen-bonded organic frameworks using triskele-shaped building units. We uncovered an unusual syn conformation of acylhydrazone, which forms hydrogen bonding with carboxyl groups, thereby allowing the rapid, scalable synthesis of a series of single crystals with exceptional stability, including resistance to aqua regia. Harnessing the enriched proton-hopping sites and acid robustness of the double-walled framework, we demonstrate that incorporating superacids into these dual-porous crystals effectively enhances proton conductivity, which reaches 4.25 × 10−3 S cm−1 at 30 °C. Furthermore, we elucidate the formation mechanism of double-walled hydrogen-bonded organic frameworks via a combination of experimental and computational approaches. This work opens avenues for the tailored design of multi-porous materials with independently tunable pore architectures and functionalities.