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首页> 外文期刊>Crystal growth & design >A novel porphyrin-based ligand containing four 4,4′-dipyridylamine moieties: Syntheses, structures, and luminescent properties of Mn(II), Cu(II), Zn(II), and Cd(II) coordination polymers
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A novel porphyrin-based ligand containing four 4,4′-dipyridylamine moieties: Syntheses, structures, and luminescent properties of Mn(II), Cu(II), Zn(II), and Cd(II) coordination polymers

机译：一种新颖的基于卟啉的配体，包含四个4,4'-联吡啶胺部分：Mn（II），Cu（II），Zn（II）和Cd（II）配位聚合物的合成，结构和发光性质

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摘要

The design and syntheses of porphyrin-based ligands are attractive for creating coordination assemblies with novel structures and intriguing properties. In this work, we designed and synthesized a novel porphyrin-based ligand 5,10,15,20-tetrakis(4,4′-dipyridylaminophenylene)porphyrin (TDPAP, H_2L) by the introduction of four peripheral 4,4′-dipyridylamine moieties to a porphyrin platform. Starting from this novel ligand, the protonated form of the ligand H_4LCl_2·2CH_3OH·2H_2O (1) and four coordination polymers [Mn(III)Mn(II)LCl_3(DMF)]_n (2), [Cu_4L(CH_3COO)_5(HCOO)(CH_3COOH)(H_2O)_3]_n·nCH_3COOH·nH_2O (3), [Zn_3L(CH_3COO)_4]_n (4), and [Cd_2H_2L(CH_3COO)_4]_n· nDMF·nCH_3COOH·2nH_2O (5) were synthesized. Single crystal X-ray diffraction analyses revealed that a rich structural diversity was observed for these compounds due to the coordination of the multiple peripheral pyridines as well as the porphyrin core. 1 displays a hydrogen bonded one-dimensional (1D) structure composed of [(H_2O)_2Cl_2]~(2-) moieties. Complex 2 shows interpenetrated two-dimensional (2D) coordination networks, which are further linked by π?π stacking interactions to afford a three-dimensional (3D) structure. 3 shows a 2D sheet composed of 50- and 70-membered metallomacrocycles. In complex 4, 1D zigzag coordination chains were generated and further linked to form a 2D structure. Complex 5 has a stairlike 2D structure formed by the linkage of 1D coordination chains through the bridging of binuclear [Cd_2(CO_2)_4] subunits. In these compounds, TDPAP shows a unique coordination behavior. It may bind 4-7 metal centers, and it demonstrates conformational flexibility and the ability to form intermolecular hydrogen bonds and π?π interactions, which contribute to the formation of novel supramolecular structures. On the basis of the novel structures, the solid state emissions of the compounds were also investigated.
机译：卟啉基配体的设计和合成对于创建具有新颖结构和引人入胜特性的配位体组件具有吸引力。在这项工作中，我们通过引入四个外围的4,4'-二吡啶基胺部分，设计并合成了一种新型的基于卟啉的配体5,10,15,20-四（4,4'-二吡啶基氨基亚苯基）卟啉（TDPAP，H_2L）到卟啉平台。从这种新型配体开始，配体H_4LCl_2·2CH_3OH·2H_2O（1）和四种配位聚合物[Mn（III）Mn（II）LCl_3（DMF）] _ n（2），[Cu_4L（CH_3COO）_5（ HCOO）（CH_3COOH）（H_2O）_3] _n·nCH_3COOH·nH_2O（3），[Zn_3L（CH_3COO）_4] _n（4）和[Cd_2H_2L（CH_3COO）_4] _n·nDMF·nCH_3COOH·2nH_2O（5）合成的。单晶X射线衍射分析显示，由于多个外围吡啶以及卟啉核的配位，这些化合物观察到了丰富的结构多样性。图1显示了由[（H_2O）_2Cl_2]〜（2-）部分组成的氢键一维（1D）结构。复合体2显示了互穿的二维（2D）协调网络，这些网络通过πππ堆叠相互作用进一步链接在一起，从而提供了三维（3D）结构。图3显示了由50和70元金属大环组成的2D薄片。在复杂的4中，生成了1D之字形协调链，并进一步链接以形成2D结构。配合物5具有阶梯状的2D结构，其通过双核[Cd_2（CO_2）_4]亚基的桥接通过一维配位链的连接而形成。在这些化合物中，TDPAP显示出独特的配位行为。它可以结合4-7个金属中心，并且显示出构象柔性以及形成分子间氢键和πππ相互作用的能力，这有助于形成新的超分子结构。在新颖结构的基础上，还研究了化合物的固态发射。

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