基于双（苯并咪唑）ZnCl2 配合物的氢键有机骨架的合成、结构表征和客体交换性能,Inorganic Chemistry

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基于双（苯并咪唑）ZnCl2 配合物的氢键有机骨架的合成、结构表征和客体交换性能
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-11-25 , DOI: 10.1021/acs.inorgchem.2c03131
Yurika Iwabuchi ₁ , Ryoga Yamaguchi ₁ , Tatsunari Murakami ₁ , Masaaki Okazaki ₁ , Shun Ohta ₁

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基于配位化合物的氢键有机骨架 (HOF) 构成了一类正在开发的有趣多孔材料。在此，我们报告了四种基于带有双（苯并咪唑基）甲烷配体（双（苯并咪唑）ZnCl ₂）的二氯化锌络合物的 HOF 的合成、晶体结构和客体交换特性。这些基于双（苯并咪唑）ZnCl ₂的 HOF 的多孔结构的主要特征在于分子间 N–H···Cl 氢键以及 π–π 相互作用。发现这些 HOF 之一通过以下方式交换客体分子有或没有结构变化的单晶到单晶的转变。单晶 X 射线衍射研究表明，伴随结构变化的客体交换是由双（苯并咪唑）ZnCl ₂配合物之间的 N–H···Cl 氢键断裂引起的，随后形成与客体分子交替形成氢键。这一结果表明，使用比通常用于构建 HOF 的氢键（例如，羧酸二聚体、N-杂环和电荷辅助部分）更弱的 N-H···Cl 氢键可能代表一种方便的合成策略灵活的 HOF。

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Synthesis, Structural Characterization, and Guest Exchange Properties of Hydrogen-Bonded Organic Frameworks Based on Bis(benzimidazole)ZnCl2 Complexes

Hydrogen-bonded organic frameworks (HOFs) based on coordination compounds constitute a developing class of interesting porous materials. Herein, we report on the synthesis, crystal structures, and guest exchange properties of four HOFs based on zinc dichlorido complexes that bear a bis(benzimidazolyl)methane ligand (bis(benzimidazole)ZnCl₂). The porous structures of these bis(benzimidazole)ZnCl₂-based HOFs are characterized predominantly by intermolecular N–H···Cl hydrogen bonds in conjunction with π–π interactions. One of these HOFs was found to exchange guest molecules via single-crystal-to-single-crystal transformations with or without structural change. A single-crystal X-ray diffraction study revealed that the guest exchange accompanied by a structural change is induced by the cleavage of the N–H···Cl hydrogen bonds between the bis(benzimidazole)ZnCl₂ complexes, followed by the formation of alternate hydrogen bonds with guest molecules. This result suggests that the use of weaker N–H···Cl hydrogen bonds than those typically used for the construction of HOFs (e.g., carboxylic acid dimers, N-heterocycles, and charge-assisted moieties) may represent a convenient strategy to synthesize flexible HOFs.

更新日期：2022-11-25

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