Ligand Defect Density Regulation in Metal–Organic Frameworks by Functional Group Engineering on Linkers,Nano Letters

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Ligand Defect Density Regulation in Metal–Organic Frameworks by Functional Group Engineering on Linkers
Nano Letters ( IF 9.6 ) Pub Date : 2022-01-10 , DOI: 10.1021/acs.nanolett.1c04574
Qihao Yang _{1,

2} , Yinming Wang _{1,

2} , Xuan Tang ₃ , Qiuju Zhang _{1,

2} , Sheng Dai ₃ , Huaitao Peng ₁ , Yichao Lin _{1,

2} , Ziqi Tian _{1,

2} , Zhiyi Lu _{1,

2} , Liang Chen _{1,

2}

Affiliation

Defects in solid materials vitally determine their physicochemical properties; however, facile regulation of the defect density is still a challenge. Herein, we demonstrate that the ligand defect density of metal–organic frameworks (MOFs) with a UiO-66 structural prototype is precisely regulated by tuning the linker groups (X = OMe, Me, H, F). Detailed analyses reveal that the ligand defect concentration is positively correlated with the electronegativity of linker groups, and Ce-UiO-66-F, constructed by F-containing ligands and Ce-oxo nodes, possesses the superior ligand defect density (>25%) and identifiable irregular periodicity. The increase in ligand defect density results in the reduction of the valence state and the coordination number of Ce sites in Ce-UiO-66-X, and this merit further validates the relationship between the defective structure and catalytic performance of CO₂ cycloaddition reaction. This facile, efficient, and reliable strategy may also be applicable to precisely constructing the defect density of porous materials in the future.

中文翻译：

金属有机框架中的配体缺陷密度调节功能组工程对接头

固体材料的缺陷决定了它们的物理化学性质；然而，缺陷密度的轻松调节仍然是一个挑战。在这里，我们证明了具有 UiO-66 结构原型的金属有机框架 (MOF) 的配体缺陷密度可以通过调整连接基团 (X = OMe, Me, H, F) 来精确调节。详细分析表明，配体缺陷浓度与连接基团的电负性呈正相关，由含F配体和Ce-oxo节点构建的Ce-UiO-66-F具有优异的配体缺陷密度（>25%）和可识别的不规则周期性。配体缺陷密度的增加导致 Ce-UiO-66-X 中 Ce 位点的价态和配位数降低，₂环加成反应。这种简便、高效、可靠的策略未来也可能适用于精确构建多孔材料的缺陷密度。

更新日期：2022-01-26

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