Influence of Semirigidity and Diverse Binding Modes of an Asymmetric Pyridine-pyrazole Based Bis-Chelating Ligand in Controlling Molecular Architectures and Their Properties,Crystal Growth & Design

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Influence of Semirigidity and Diverse Binding Modes of an Asymmetric Pyridine-pyrazole Based Bis-Chelating Ligand in Controlling Molecular Architectures and Their Properties
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2020-07-29 , DOI: 10.1021/acs.cgd.9b01496
Sukhen Bala _{1,

2} , Avik De ₁ , Amit Adhikary ₁ , Sayan Saha ₁ , Sohel Akhtar ₁ , Krishna Sundar Das ₁ , Ming-Liang Tong ₂ , Raju Mondal ₁

Affiliation

We report herein the synthesis, characterization, and properties of some metal directed architectures using a new asymmetric, semirigid, and bis-chelating pyridine-pyrazole based ligand, {N′-(amino (pyrimidin-2-yl)methylene)-3-(pyridin-2-yl)-1H-pyrazole-5-carbohydrazide (H₂APPC)}. The H₂APPC ligand forms multinuclear cage complexes with different transition metal salts ranging from discrete mononuclear complex to nonanuclear with different kinds of network topologies. The semirigid ligand molecule not only changes the conformation but also exhibits variable coordination behavior, depending on the metal ions used. For instance, the reaction of manganese salt with H₂APPC results in a truncated [3 × 3] grid network, whereas the nickel salt forms a highly unusual hexanuclear cage complex. Interestingly, in the presence of copper salt, H₂APPC forms a different kind of structure along with an in situ generated new ligand. The zinc salts form a mononuclear complex. Most interestingly, reaction with cadmium salts leads to an intriguing [3 × 3] grid network, with a highly unusual occurrence of multiple variants of coordination environments around the metal centers. It is imperative to note here that the above display of metal-directed architectures is quite uncommon for an asymmetric semirigid ligand and cadmium complex that shows four kinds of coordination geometries which are not known in the literature, to the best of our knowledge. The variable temperature magnetic measurements of manganese, nickel, and copper complex showed strong antiferromagnetic interactions between the neighboring metal centers. Furthermore, the Cd₉ framework showed promising solvent-dependent luminescent properties.

中文翻译：

半刚性和不同结合方式的不对称吡啶-吡唑基双螯合配体在控制分子结构中的作用及其性能

我们在这里报告了使用新的不对称，半刚性和双螯合吡啶-吡唑基配体{ N '-（氨基（嘧啶-2-基）亚甲基）-3-的金属定向结构的合成，表征和性质（吡啶-2-基）-1 H-吡唑-5-碳酰肼（H ₂ APPC）}。H ₂ APPC配体形成具有不同过渡金属盐的多核笼络合物，过渡金属盐的范围从离散的单核络合物到具有不同网络拓扑结构的非核盐。取决于所使用的金属离子，半刚性配体分子不仅改变构象，而且表现出可变的配位行为。例如，锰盐与H ₂的反应APPC导致截断的[3×3]网格网络，而镍盐形成了高度不寻常的六核笼状复合物。有趣的是，在铜盐存在下，H ₂APPC与原位生成的新配体一起形成另一种结构。锌盐形成单核络合物。最有趣的是，与镉盐的反应导致了一个引人入胜的[3×3]网格网络，在金属中心周围非常罕见地出现了多种不同的配位环境。在此必须注意的是，对于不对称的半刚性配体和镉络合物而言，上述显示的金属定向结构非常罕见，据我们所知，它显示了文献中未知的四种配位几何。锰，镍和铜配合物的可变温度磁测量结果显示，相邻金属中心之间存在强反铁磁相互作用。此外，Cd ₉ 框架显示出有前途的溶剂依赖性发光特性。

更新日期：2020-09-02

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