<br>基于MOF-on-MOF分层结构的传感单元和吸附基团的分离，用于高灵敏度检测和去除Hg2+,Inorganic Chemistry

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基于MOF-on-MOF分层结构的传感单元和吸附基团的分离，用于高灵敏度检测和去除Hg2+
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-01-12 , DOI: 10.1021/acs.inorgchem.3c04177
Xiaoya Bi ₁ , Xiaohong Liu ₁ , Lijun Luo ₁ , Shuda Liu ₁ , Yi He ₁ , Li Zhang ₁ , Libo Li _{1,

2} , Tianyan You _{1,

3}

Affiliation

双功能材料由于其两种功能的集成而引起了污染物检测和去除领域的持续关注，但它们通常仅在这两个方面之一表现出卓越的性能。双功能材料的两个功能单元之间的相互作用可能会损害它们的传感和吸附能力。在域构建块（DBB）概念的指导下，通过在金属有机框架（MOF）上生长金纳米簇（AuNC）嵌入沸石咪唑酯框架8（AuNCs / ZIF-8）来设计分层金属有机框架（MOF）-MOF杂化物。 Zr-MOF (UiO-66-NH ₂ ) 表面用于同时检测和去除 Hg ²⁺ 。在杂化物中，氨基（-NH ₂ ）和AuNCs—分别是吸附基团和传感单元，是彼此隔离的。具体而言，吸附基团（-NH ₂ ）组装在内UiO-66-NH ₂层中，而传感单元（AuNC）被限制在外ZIF-8层中。这种分层结构不仅在空间上阻碍了这两个单元之间的电子转移，而且由于ZIF-8对AuNCs的限制而引发了AuNCs的聚集诱导发射，从而使AuNCs的荧光从猝灭变为增强。正如预期的那样，新制备的 UiO-66-NH ₂ @AuNCs/ZIF-8 杂化物对 Hg ²⁺显示出超低的检测限（0.42 ppb）和高吸附容量（129.9 mg·g ^–1 ）。总的来说，这项工作为提高基于 DBB 的 MOF 复合材料的综合性能提供了一种可行的方法。

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Isolation of Sensing Units and Adsorption Groups Based on MOF-on-MOF Hierarchical Structure for Both Highly Sensitive Detection and Removal of Hg2+

Bifunctional materials have attracted ongoing interest in the field of detection and removal of contaminants because of their integration of two functions, but they exhibit commonly exceptional performance in only one of these two aspects. The interaction between the two functional units of the bifunctional materials may compromise their sensing and adsorption abilities. Guided by the concept of domain building blocks (DBBs), a hierarchical metal–organic framework (MOF)-on-MOF hybrid was designed by growing gold nanoclusters (AuNCs)-embedded zeolitic imidazolate framework 8 (AuNCs/ZIF-8) on the surface of Zr-MOF (UiO-66-NH₂) for the simultaneous detection and removal of Hg²⁺. In the hybrid, the amino groups (−NH₂) and AuNCs─which were the adsorption groups and sensing units, respectively, were isolated from each other. Specifically, the adsorption groups (−NH₂) were assembled in the inner UiO-66-NH₂ layer, while the sensing units (AuNCs) were confined in the outer ZIF-8 layer. This hierarchical structure not only spatially hindered the electron transfer between these two units but also triggered the aggregation-induced emission of AuNCs because of the confinement of ZIF-8 on the AuNCs, thus changing the fluorescence of AuNCs from quenching to enhancement. The newly prepared UiO-66-NH₂@AuNCs/ZIF-8 hybrid, as expected, showed an ultralow detection limit (0.42 ppb) and a high adsorption capacity (129.9 mg·g^–1) for Hg²⁺. Overall, this work provides a feasible approach to improve the integrated performance of MOF-based composites based on DBBs.

更新日期：2024-01-12

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