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<p>The deliberate control of framework dimensionality represents a powerful yet underexplored strategy for tailoring the functionality of homochiral metal-organic frameworks (HMOFs). Herein, we report a logical dimensional evolution from 1D and 2D to 3D HMOFs, achieved by tuning the connectivity of the auxiliary ligand. Employing a planar, three-connected ligand, 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (Tpt), together with enantiopure tetracarboxylate of cyclohexane diamide linkers ((1<i>R</i>,2<i>R</i>/1<i>S</i>,2<i>S</i>)-cyclohexane-1,2-dicarbonyl bis(azanediyl)diisophthalate) (<i>R</i>,<i>R</i>/<i>S</i>,<i>S</i>-CHCAIP) and Zn<sup>2+</sup> salts, a pair of 3D porous HMOFs (<i>P/M</i>-HMOF-5) was successfully constructed. The 3D framework features unique heart-shaped channels and a novel 4-(3,3,3,6)-connected topology. Structural analyses reveal trinuclear Zn<sub>3</sub>(<i>μ</i><sub>3</sub>-O) clusters that, upon activation, generate open metal sites. These Lewis acid sites, synergizing with Lewis basic sites from the framework, confer efficient acid-base bifunctional heterogeneous catalysis for the synthesis of 2,3-dihydroquinazolinones in excellent yields (90%–98%). Furthermore, <i>P/M</i>-HMOF-5 serve as highly sensitive and enantioselective fluorescent sensors for amino acids and α-hydroxy carboxylic acids, with the highest discrimination observed for phenylalanine (KBH<sub>(<i>D</i>-Phe)</sub>/KBH<sub>(<i>L</i>-Phe)</sub> = 5.85 for <i>M</i>-HMOF-5). This work demonstrates how rational ligand connectivity steers dimensional evolution, enabling the integration of distinct catalytic and sensing functions within a single chiral platform, thereby providing a blueprint for the design of advanced multifunctional materials.</p>

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Dimensionally extended homochiral MOFs for catalysis and enantioselective sensing

  • 期刊论文

  • 发表日期：

    2026年3月2日

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  • Yan-Wu Zhao,
  • Sheng-Yan Zhu,
  • Zhi-Hang Li,
  • Xiao-Jian Han,
  • Nan Zhang,
  • Mei Pan,
  • Xian-Ming Zhang

摘要

The deliberate control of framework dimensionality represents a powerful yet underexplored strategy for tailoring the functionality of homochiral metal-organic frameworks (HMOFs). Herein, we report a logical dimensional evolution from 1D and 2D to 3D HMOFs, achieved by tuning the connectivity of the auxiliary ligand. Employing a planar, three-connected ligand, 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (Tpt), together with enantiopure tetracarboxylate of cyclohexane diamide linkers ((1R,2R/1S,2S)-cyclohexane-1,2-dicarbonyl bis(azanediyl)diisophthalate) (R,R/S,S-CHCAIP) and Zn2+ salts, a pair of 3D porous HMOFs (P/M-HMOF-5) was successfully constructed. The 3D framework features unique heart-shaped channels and a novel 4-(3,3,3,6)-connected topology. Structural analyses reveal trinuclear Zn3(μ3-O) clusters that, upon activation, generate open metal sites. These Lewis acid sites, synergizing with Lewis basic sites from the framework, confer efficient acid-base bifunctional heterogeneous catalysis for the synthesis of 2,3-dihydroquinazolinones in excellent yields (90%–98%). Furthermore, P/M-HMOF-5 serve as highly sensitive and enantioselective fluorescent sensors for amino acids and α-hydroxy carboxylic acids, with the highest discrimination observed for phenylalanine (KBH(D-Phe)/KBH(L-Phe) = 5.85 for M-HMOF-5). This work demonstrates how rational ligand connectivity steers dimensional evolution, enabling the integration of distinct catalytic and sensing functions within a single chiral platform, thereby providing a blueprint for the design of advanced multifunctional materials.