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<p>Zirconium metal-organic frameworks (Zr-MOFs) have garnered significant attention due to their outstanding stability and structural designability. However, research on Zr-MOFs constructed with desymmetric ligands remains scarce, largely constrained by the geometric symmetry limitations of the employed ligands. To further expand the structural diversity of Zr-MOFs, two novel Zr-MOFs, <b>JLU-MOF311</b> {[Zr<sub>6</sub>(<i>μ</i>-O)<sub>4</sub>(<i>μ</i>-OH)<sub>4</sub>(OH)<sub>3</sub>(H<sub>2</sub>O)<sub>3</sub>(COOH)]<sub>2</sub>(Iso-TBCIDC)<sub>4</sub>} and <b>JLU-MOF312</b> {Zr<sub>6</sub>(<i>μ</i>-O)<sub>4</sub>(<i>μ</i>-OH)<sub>4</sub>(OH)<sub>4</sub>(H<sub>2</sub>O)<sub>4</sub>(Iso-TBCBIDC)<sub>2</sub>} were successfully synthesized (Iso-H<sub>4</sub>TBCIDC = 2′-(4,5-bis(4-carboxyphenyl)-1H-imidazol-2-yl)-[1,1′:4′,1″-terphenyl]-4,4″-dicarboxylic acid; Iso-H<sub>4</sub>TBCBIDC = 2′-(4,5-bis(4′-carboxy-[1,1′-biphenyl]-4-yl)-1H-imidazol-2-yl)-[1,1′:4′,1″-terphenyl]-4,4″-dicarboxylic acid) by ligand desymmetry strategy. <b>JLU-MOF311</b> and <b>JLU-MOF312</b> with unprecedented (4,8)-connected topological structures exhibit significant fluorescence turn-on responses to perfluorooctanoic acid (PFOA) with detection limits in aqueous solutions as low as 22.8 nM and 0.24 µM, respectively. <b>JLU-MOF311</b> constructed by the (Zr<sub>6</sub>)<sub>2</sub> cluster exhibits more open sites than <b>JLU-MOF312</b> built by the Zr<sub>6</sub> cluster. <b>JLU-MOF311</b> demonstrates higher sensitivity toward PFOA, a finding further validated by density functional theory (DFT) calculations. This work demonstrates that, guided by reticular chemistry, the desymmetrization of ligands enables the synthesis of Zr-MOFs with non-default topologies, for the detection of low-concentration PFOA. This approach also provides a novel pathway for highly sensitive detection of perfluoroalkyl substances and other polyfluoroalkyl substances.</p>

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Pre-designed asymmetric ligands for assembling Zr-MOFs toward highly efficient turn-on fluorescent detection of perfluorooctanoic acid

  • 期刊论文

  • 发表日期：

    2026年5月22日

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  • Jincheng Si,
  • Yifeng Xue,
  • Kang Zhou,
  • Kaiyue Liu,
  • Chenbo Li,
  • Zhaoyuan Zhang,
  • Mingyue Qiu,
  • Shuyu Xie,
  • Xueliang Qin,
  • Hailun Xia,
  • Xiao-Yuan Liu,
  • Yunling Liu

摘要

Zirconium metal-organic frameworks (Zr-MOFs) have garnered significant attention due to their outstanding stability and structural designability. However, research on Zr-MOFs constructed with desymmetric ligands remains scarce, largely constrained by the geometric symmetry limitations of the employed ligands. To further expand the structural diversity of Zr-MOFs, two novel Zr-MOFs, JLU-MOF311 {[Zr6(μ-O)4(μ-OH)4(OH)3(H2O)3(COOH)]2(Iso-TBCIDC)4} and JLU-MOF312 {Zr6(μ-O)4(μ-OH)4(OH)4(H2O)4(Iso-TBCBIDC)2} were successfully synthesized (Iso-H4TBCIDC = 2′-(4,5-bis(4-carboxyphenyl)-1H-imidazol-2-yl)-[1,1′:4′,1″-terphenyl]-4,4″-dicarboxylic acid; Iso-H4TBCBIDC = 2′-(4,5-bis(4′-carboxy-[1,1′-biphenyl]-4-yl)-1H-imidazol-2-yl)-[1,1′:4′,1″-terphenyl]-4,4″-dicarboxylic acid) by ligand desymmetry strategy. JLU-MOF311 and JLU-MOF312 with unprecedented (4,8)-connected topological structures exhibit significant fluorescence turn-on responses to perfluorooctanoic acid (PFOA) with detection limits in aqueous solutions as low as 22.8 nM and 0.24 µM, respectively. JLU-MOF311 constructed by the (Zr6)2 cluster exhibits more open sites than JLU-MOF312 built by the Zr6 cluster. JLU-MOF311 demonstrates higher sensitivity toward PFOA, a finding further validated by density functional theory (DFT) calculations. This work demonstrates that, guided by reticular chemistry, the desymmetrization of ligands enables the synthesis of Zr-MOFs with non-default topologies, for the detection of low-concentration PFOA. This approach also provides a novel pathway for highly sensitive detection of perfluoroalkyl substances and other polyfluoroalkyl substances.