覆盆子形MOF@MOF的构建与传感放大,Inorganic Chemistry

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覆盆子形MOF@MOF的构建与传感放大
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-03-10 , DOI: 10.1021/acs.inorgchem.1c04027
Ming-Xue Wu ₁ , Chunlei Wei _{1,

2} , Xing-Huo Wang ₁ , Qing-Qing Xia ₁ , Huiqi Wang ₃ , Xiaomin Liu ₁

Affiliation

MOFs@MOFs（金属-有机框架，MOFs）具有精确的定制功能和预先设计的结构，与传统的单一 MOFs 相比，能够针对特定功能实施结构和性能调节。然而，多层MOFs@MOFs的合成和荧光性能仍有待改进。在此，通过优化种子介导合成，通过调整反应时间、反应模式和反应浓度，构建了一种荧光覆盆子形 MOF@MOF，包括 UiO-66-NH ₂核的初始合成和涂层的涂层。 UiO-67-bpy 外壳。覆盆子状的 UiO-66@67-bpy 对 Hg ^{2+表现出稳定的荧光和理想的传感选择性}离子在其他离子的干扰下；同时，覆盆子状的 UiO-66@67-bpy 比纯 UiO-66-NH ₂、机械混合的 UiO-66-NH ₂ + UiO-67-bpy 和 UiO-66@UiO-67表现出增强的传感性能由于外层 UiO-67-bpy 对 Hg ²⁺的积累作用。密度泛函理论 (DFT) 计算包括吸附能计算和电子密度差分析进一步表明，增强的荧光猝灭可能归因于外部 UiO-67-bpy 富集促进 Hg ^{2+之间的电荷转移}和荧光 UiO-66@67-bpy 的配体。MOFs@MOFs 的协同效应为构建增强型传感器和其他应用提供了更多可能性。

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Construction and Sensing Amplification of Raspberry-Shaped MOF@MOF

MOFs@MOFs (metal–organic frameworks, MOFs) possess precise customized functionalities and predesigned structures that enable the implementation of structure and property regulation for specific functions in comparison to traditional single MOFs. However, the synthesis and fluorescence properties of multilayer MOFs@MOFs are still worth improving. Herein, a fluorescent raspberry-shaped MOF@MOF was constructed via optimized seed-mediated synthesis by tuning the reaction time, reaction mode, and reaction concentration, involving the initial synthesis of the UiO-66-NH₂ core and then the coating of the UiO-67-bpy shell. The raspberry-shaped UiO-66@67-bpy showed stable fluorescence and desirable sensing selectivity for the Hg²⁺ ion under the interference of other ions; meanwhile, the raspberry-shaped UiO-66@67-bpy indicated amplified sensing performance than pure UiO-66-NH₂, mechanically mixed UiO-66-NH₂ + UiO-67-bpy, and UiO-66@UiO-67 counterpart due to the accumulation effect of outer UiO-67-bpy toward Hg²⁺. Density functional theory (DFT) calculations including adsorption energy calculations and electronic density difference analysis further showed that the enhanced fluorescence quenching was possibly attributed to the outer UiO-67-bpy enrichment promoting the charge transfer between Hg²⁺ and the ligands of fluorescent UiO-66@67-bpy. The synergistic effect of MOFs@MOFs unlocks more possibilities for the construction of enhanced sensors and other applications.

更新日期：2022-03-10

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