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首页> 外文期刊>Crystal growth & design >Novel bis(4,4′-dipyridylamine) ligand with a flexible butadiyne linker: Syntheses, structures, and photoluminescence of d ~(10) metal coordination polymers
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Novel bis(4,4′-dipyridylamine) ligand with a flexible butadiyne linker: Syntheses, structures, and photoluminescence of d ~(10) metal coordination polymers

机译：具有柔性丁二炔接头的新型双（4,4'-二吡啶胺）配体：d〜（10）金属配位聚合物的合成，结构和光致发光

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摘要

The design and syntheses of novel ligands are essential for developing coordination compounds with novel structures and interesting properties. In this work, we designed and synthesized a novel ligand bis(4,4′- dipyridylaminophenylene)butadiyne (L) by attaching two 4,4′-dipyridylamine moieties to a flexible butadiyne linker. Starting from this novel ligand, seven coordination polymers [Zn _2L(HCOO) _3(OH)] _n (1), [Cd _2L _2Cl _4] _n?3nDMF?3nH _2O (2), [CdLBr _2] _n (3), [Cd _6L _3(SO _4) _6] _n?4nMeCN (4), [Hg _2LBr _4] _n?3nCH _2Cl _2?nH _2O (5), [Cu _2LI _2] n?0.5nCH _2Cl _2 (6), and [Ag _2L(H _2O) _2] _n(NO _3) _(2n)?2nH _2O (7) were synthesized. Single-crystal X-ray diffraction analyses revealed that two forms of the ligand crystals, L and L?0.5DMF present straight and bent conformations, respectively, because of the flexibility of the butadiyne unit. A rich structural diversity was observed for its d ~(10) metal complexes. Complexes 1 and 5 present ladder-like structures. In complexes 2 and 4, the ligand molecules are linked by metal atoms to afford 3D supramolecular structures. It is noteworthy that the 3D structure of complex 4 consists of interesting infinite {Cd _6(SO _4) _6} _∞ chains, whereas complexes 3, 6, and 7 exhibit 2D network structures. Interestingly, in the crystal of complex 7, each ligand links four metal ions and each Ag ion bridges two ligands, leading to the formation of undulated 2D sheets with large cavities composed of 66-membered metallomacrocycles, which are interpenetrated by three other such 2D sheets, affording a 4-fold interpenetrated structure. In summary, the complex structures are dependent on the metal ions and the anions. In addition, the flexibility of the butadiyne moiety provides additional means for modulating the structures. Solid state photoluminescence of the free ligand and the complexes shows emission maxima within the range of 420-515 nm, which can be modulated by the conformations of the ligand in addition to the variation of the metal ions and anions, and the introduction of the butadiyne unit has a bathochromic effect.
机译：新型配体的设计和合成对于开发具有新型结构和有趣特性的配位化合物至关重要。在这项工作中，我们通过将两个4,4'-二吡啶基胺部分连接到柔性丁二炔接头上，设计并合成了一种新型配体双（4,4'-二吡啶基氨基亚苯基）丁二炔（L）。从这种新型配体开始，七个配位聚合物[Zn _2L（HCOO）_3（OH）] _n（1），[Cd _2L _2Cl _4] _n？3nDMF？3nH _2O（2），[CdLBr _2] _n（3） [Cd _6L _3（SO _4）_6] _n？4nMeCN（4），[Hg _2LBr _4] _n？3nCH _2Cl _2？nH _2O（5），[Cu _2LI _2] n？0.5nCH _2Cl _2（6）和合成了[Ag _2L（H _2O）_2] _n（NO _3）_（2n）→2nH _2O（7）。单晶X射线衍射分析表明，由于丁二炔单元的柔韧性，配体晶体的两种形式，L和L≥0.5DMF分别呈现出直的和弯曲的构象。观察到其d〜（10）金属配合物具有丰富的结构多样性。配合物1和5呈现梯状结构。在络合物2和4中，配体分子通过金属原子连接以提供3D超分子结构。值得注意的是，复合物4的3D结构由有趣的无限{Cd _6（SO _4）_6}_∞链组成，而复合物3、6和7则显示2D网络结构。有趣的是，在配合物7的晶体中，每个配体连接四个金属离子，每个Ag离子桥接两个配体，导致形成具有由66元金属大环组成的大空腔的起伏的2D薄板，这些薄板由其他三个此类2D薄板互穿，提供4倍互穿结构。总之，复杂的结构取决于金属离子和阴离子。另外，丁二炔部分的柔韧性提供了调节结构的其他手段。游离配体和配合物的固态光致发光显示最大发射在420-515 nm范围内，除了金属离子和阴离子的变化以及丁二炔的引入外，还可以通过配体的构象进行调节单位具有红移作用。

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