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<p>Hierarchical metal–organic framework (HS-MOF) films have attracted considerable attention due to their enhanced mass transport, larger accessible surface area, and superior performance in catalysis, separation, and sensing compared to conventional dense MOF films. However, the controlled fabrication of such hierarchical MOF films remains challenging. In this work, we present a facile and effective modulator-assisted strategy for the direct fabrication of hierarchical ZIF-8 films on bare Al substrates. By introducing stearic acid as a multifunctional modulator, we successfully orchestrate both the chemical environment and the growth kinetics during ZIF-8 crystallization. Stearic acid is proposed to play a dual role in ZIF-8 crystallization. It could serve as dynamic proton regulator, shifting the deprotonation equilibrium of 2-methylimidazole to control ligand availability and suppress homogeneous nucleation. Simultaneously, it serves as a competitive coordination ligand, forming transient zinc stearate complexes, which can buffer the release of zinc ions and guide the growth of hierarchical structures. This coordinated regulatory mechanism is suggested to not only inhibit the homogeneous crystallization process but also promote the directional heterogeneous growth of the substrate, thereby forming ZIF-8 films with tunable nanopore to micropore scales. Furthermore, the proposed strategy is also applicable to Zn substrate, providing a potential route for designing advanced MOF-based functional coatings.</p>

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Direct fabrication of metal–organic frameworks films with hierarchical structures by the modulation of ligand competitors

  • 期刊论文

  • 发表日期：

    2026年5月3日

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  • Xiaofeng Ding,
  • Jinjie Liu,
  • Xilong Hao,
  • Yuezhong Zhang,
  • Fuqiang Zhao,
  • Dongshi Xu,
  • Xinyuan Wei,
  • Xuan Zhang

摘要

Hierarchical metal–organic framework (HS-MOF) films have attracted considerable attention due to their enhanced mass transport, larger accessible surface area, and superior performance in catalysis, separation, and sensing compared to conventional dense MOF films. However, the controlled fabrication of such hierarchical MOF films remains challenging. In this work, we present a facile and effective modulator-assisted strategy for the direct fabrication of hierarchical ZIF-8 films on bare Al substrates. By introducing stearic acid as a multifunctional modulator, we successfully orchestrate both the chemical environment and the growth kinetics during ZIF-8 crystallization. Stearic acid is proposed to play a dual role in ZIF-8 crystallization. It could serve as dynamic proton regulator, shifting the deprotonation equilibrium of 2-methylimidazole to control ligand availability and suppress homogeneous nucleation. Simultaneously, it serves as a competitive coordination ligand, forming transient zinc stearate complexes, which can buffer the release of zinc ions and guide the growth of hierarchical structures. This coordinated regulatory mechanism is suggested to not only inhibit the homogeneous crystallization process but also promote the directional heterogeneous growth of the substrate, thereby forming ZIF-8 films with tunable nanopore to micropore scales. Furthermore, the proposed strategy is also applicable to Zn substrate, providing a potential route for designing advanced MOF-based functional coatings.