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Lanthanide Molecular Clusters and Metal–Organic Layers Constructed by Manipulation of Substituents

化学 镧系元素 金属 立体化学 结晶学 计算化学 有机化学 离子
作者
Yun‐Lan Li,Hai‐Hang Lan,Hai‐Ling Wang,Zhong‐Hong Zhu,Lei Cheng,Hua‐Hong Zou
出处
期刊:Inorganic Chemistry [American Chemical Society]
标识
DOI:10.1021/acs.inorgchem.4c04885
摘要

Usually, complexes with different connections and shapes are constructed by regulating the substituents. However, it is extremely challenging to construct two lanthanide complexes with different dimensions by only fine-tuning the substituents of the ligands, especially the substituents (−CH3 and −CH2CH3) with almost similar physical and chemical properties. Herein, by only regulating the substituents of the multidentate chelating ligands, two lanthanide complexes with different dimensions and connection modes were successfully constructed using a multicomponent "one-pot method" under the guidance of the multidentate chelating coordination method (MCC). They are the 11-nuclear lanthanide molecular cluster (Dy11) and the metal–organic layer (2D-Dy). Specifically, when the selected ligand is an imidazole-2-carboxaldehyde derivative and its substituent is −CH3, a layered 2D-Dy is obtained. The linker [Dy(HL1)3] with a propeller configuration is formed by chelating the Dy(III) ion with an acylhydrazone ligand (HL1) formed by the condensation of three salicylhydrazides and 1-methyl-1H-imidazole-2-carboxaldehyde. The above linkers were further linked alternately with propeller-shaped [Dy(NO3)3] as a secondary building unit (SBU) to form 2D-Dy. In addition, by changing the −CH3 on the ligand to −CH2CH3, we obtained an example of Dy11 formed by epitaxial assembly of two Dy(III) ions with an hourglass-shaped Dy9 as the core, and its molecular formula is [Dy11(HL2)8(μ3–OH)8(μ4-O)2(CH3O)4(NO3)4](NO3)5 18CH3OH. The cluster Dy11 was bombarded using high-resolution electrospray ionization mass spectrometry (HRESI-MS) and the molecular ion peaks of various fragments formed were captured. Based on the above molecular ion peaks, the possible fragmentation mechanisms of Dy11 were inferred to be Dy11 → Dy4(HL2)4 → Dy3(HL2)2 → Dy2(HL2)2 → Dy(HL2)2 and Dy11 → Dy(HL2)2/Dy2(HL2)2/Dy3(HL2)2/Dy4(HL2)4. This work is one of the rare examples where fine-tuning of ligand substituents leads to the formation of complexes of different dimensions, which promotes the progress of crystal engineering of lanthanide complexes.
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