Six novel coordination polymers based on the 5-(1H-tetrazol-5-yl)isophthalic acid ligand: structures, luminescence, and magnetic properties†,CrystEngComm

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Six novel coordination polymers based on the 5-(1H-tetrazol-5-yl)isophthalic acid ligand: structures, luminescence, and magnetic properties†
CrystEngComm ( IF 2.6 ) Pub Date : 2018-02-22 00:00:00 , DOI: 10.1039/c8ce00030a
Xiu-Mei Zhang _{1,

2,

3,

4,

5} , Feng Liu _{1,

2,

3,

4} , Wei Gao _{1,

2,

3,

4} , Hong Huang _{1,

2,

3,

4} , Jie-Ping Liu _{1,

2,

3,

4}

Affiliation

Six new coordination polymers (CPs), namely, [Mn₂(OH)(TZI)(DMA)] (1), [Cu₂(OH)(TZI)(DMA)]·3.5H₂O (2), [Co₂(OH)(TZI)(H₂O)₂] (3), [Zn₂(OH)(TZI)(2,2′-bpy)]·H₂O (4), [Zn₂(OH)(TZI)(phen)]·2H₂O (5) and [Zn₂(OH)(TZI)(4,4′-bpy)_0.5] (6), (H₃TZI = 5-(4-(tetrazol-5-yl)phenyl)isophthalic acid, 2,2′-bpy = 2,2′-bipyridine, phen = 1,10-phenanthroline, 4,4′-bpy = 4,4′-bipyridine, and DMA = N,N-dimethylacetamide), have been synthesized under solvo-/hydrothermal conditions. Both 1 and 2 exhibit 3D structures containing butterfly-shaped tetranuclear M₄(μ₃-OH)₂ clusters as secondary building units (SBUs). In 1, the SBUs are connected into 1D chains by the tetrazolate groups of the TZI ligands and the chains are further interlinked into a (4,8)-connected 3D net by the TZI spacers. In 2, the SBUs are directly connected by TZI to give a (3,6)-connected 3D framework. CP 3 features a double-layered structure based on corner-sharing Co₃(μ₃-OH) triangle Δ-chains in which Co(II) ions are bridged by mixed (μ₄-tetrazolate)(μ₃-OH)(μ₂-COO) bridges. CPs 4–6 were synthesized by the reactions of the H₃TZI ligands, Zn(NO₃)₂ and three different N-donor auxiliary ligands. The auxiliary ligands change from chelating ligands (2,2′-bpy, phen) to 4,4′-bpy, which leads to remarkable structural changes from 2D to 3D. CPs 4 and 5 display 2D structures with dinuclear motifs as SBUs. In 4, the dinuclear motifs with mixed double (μ₂-tetrazolate)(μ₂-OH) bridges are connected by the TZI spacers to produce a 2D framework. Differently, in 5, the dinuclear motifs with mixed double (μ₂-COO)(μ₂-OH) bridges are interlinked into a 2D framework with a (4,4)-connected net topology. In 6, the square Zn₄O₄ clusters are interlinked by the organic ligands into a 3D framework with a (4,10)-connected (4⁴·6²)(4¹²·5⁸·6¹⁶·7⁶·8³) topology. Magnetic studies indicate that CPs 1–3 exhibit antiferromagnetic coupling. Further magnetic measurement demonstrates that CPs 1 and 3 show no magnetic ordering above 2 K. CPs 4–6 exhibit strong luminescence with different energies in the solid state at room temperature.

中文翻译：

基于5-（1 H-四唑-5-基）间苯二甲酸配体的六种新型配位聚合物：结构，发光和磁性†

六种新的配位聚合物（CPs），即[Mn ₂（OH）（TZI）（DMA）]（1），[Cu ₂（OH）（TZI）（DMA）]·3.5H ₂ O（2），[ Co ₂（OH）（TZI）（H ₂ O）₂ ]（3），[Zn ₂（OH）（TZI）（2,2'-bpy）]·H ₂ O（4），[Zn ₂（OH））（TZI）（phen）]·2H ₂ O（5）和[Zn ₂（OH）（TZI）（4,4'-bpy）_0.5 ]（6），（H ₃TZI = 5-（4-（四唑-5-基）苯基）间苯二甲酸，2,2'-bpy = 2,2'-联吡啶，phen = 1,10-菲咯啉，4,4'-bpy = 4，在溶剂-/水热条件下已经合成了4'-联吡啶，并且DMA = N，N-二甲基乙酰胺。既1和2显示出含有蝴蝶形四核中号3D结构₄（μ ₃ -OH）₂簇次级结构单元（的SBU）。在图1中，SBU通过TZI配体的四唑酸酯基团连接成一维链，并且这些链通过TZI间隔基进一步互连成（4,8）连接的3D网。在2，SBU通过TZI直接连接以提供（3,6）连接的3D框架。CP 3设有基于角共享一个双层结构共₃（μ ₃ -OH）三角形Δ链，其中的Co（II）离子被混合（μ桥接₄ -tetrazolate）（μ ₃ -OH）（μ ₂ -COO）桥。CP 4–6是通过H ₃ TZI配体，Zn（NO ₃）₂和三种不同的N供体辅助配体的反应合成的。辅助配体从螯合配体（2,2'-bpy，phen）变为4,4'-bpy，这导致了从2D到3D的显着结构变化。CP 4和图5显示具有双核基序的2D结构作为SBU。在4，双核基序用混合双（μ ₂ -tetrazolate）（μ ₂ -OH）桥由TZI间隔物连接，以产生2D框架。不同地，在5，双核基序用混合双（μ ₂ -COO）（μ ₂ -OH）桥相通成具有（4,4）一个2D框架-连接网的拓扑结构。在6中，方形Zn ₄ O ₄簇通过有机配体相互连接成3D骨架，并具有（4,10）连接的（4 ⁴ ·6 ²）（4 ¹² ·5 ⁸ ·6 ¹⁶·7 ⁶ ·8 ³）拓扑。磁性研究表明，CP 1-3表现出反铁磁耦合。此外磁测量表明，CP的1和3示出上述2 K. CP的无磁有序4-6显示出在室温下以固体状态不同能量强发光。

更新日期：2018-02-22

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