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<p>Zeolites exhibit promising CO<sub>2</sub> capture capabilities but face practical challenges such as competitive water adsorption and limited selectivity. Conventional surface modifications often cause pore blockage, further complicating the balance between adsorption capacity and selectivity. In this work, we innovatively propose a COF-shell coating strategy that enables dual modulation of the surface hydrophobicity and interfacial pore aperture of zeolites. A cation-mediated <i>in-situ</i> interfacial anchoring approach is developed, utilizing NH<Stack> <sub>4</sub> <sup>+</sup> </Stack> ions on 4A zeolite to direct the oriented growth of a hydrophobic COF shell without traditional linkers. The resulting core-shell 4A@TbPa-CF<sub>3</sub> adsorbent overcomes the trade-off between capacity and selectivity, achieving a high CO<sub>2</sub> uptake of 2.86 mmol g<sup>−1</sup> and a CO<sub>2</sub>/N<sub>2</sub> selectivity of 123.6, among the best reported for zeolite-based materials. It also maintains robust performance under humid and simulated industrial flue gas conditions. This linker-free strategy resolves the fundamental challenge of inorganic-organic interfacial compatibility, representing the first successful <i>in-situ</i> nucleation and growth of a COF shell on zeolite. The dual surface-interface modification offers a new design principle for developing high-performance solid adsorbents with simultaneous high capacity and high selectivity, paving the way toward practical CO<sub>2</sub> capture from complex flue gases.</p>

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Linker-free synthesis of zeolite@COF core-shell adsorbents via dual surface-interface engineering for high-performance CO2 capture

  • 期刊论文

  • 发表日期：

    2026年5月28日

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  • Jinrong Lu,
  • Zhaoxiang Yang,
  • Xiaoxue Zhang,
  • Qiao Zhao,
  • Jijie Zhang,
  • Weijia An,
  • Li Liu,
  • Yinghua Liang,
  • Sheng Zhang,
  • Xiao Wang,
  • Wenquan Cui

摘要

Zeolites exhibit promising CO2 capture capabilities but face practical challenges such as competitive water adsorption and limited selectivity. Conventional surface modifications often cause pore blockage, further complicating the balance between adsorption capacity and selectivity. In this work, we innovatively propose a COF-shell coating strategy that enables dual modulation of the surface hydrophobicity and interfacial pore aperture of zeolites. A cation-mediated in-situ interfacial anchoring approach is developed, utilizing NH 4 + ions on 4A zeolite to direct the oriented growth of a hydrophobic COF shell without traditional linkers. The resulting core-shell 4A@TbPa-CF3 adsorbent overcomes the trade-off between capacity and selectivity, achieving a high CO2 uptake of 2.86 mmol g−1 and a CO2/N2 selectivity of 123.6, among the best reported for zeolite-based materials. It also maintains robust performance under humid and simulated industrial flue gas conditions. This linker-free strategy resolves the fundamental challenge of inorganic-organic interfacial compatibility, representing the first successful in-situ nucleation and growth of a COF shell on zeolite. The dual surface-interface modification offers a new design principle for developing high-performance solid adsorbents with simultaneous high capacity and high selectivity, paving the way toward practical CO2 capture from complex flue gases.