萘二酸、吡嗪与过渡金属锰、铜、锌配位聚合物的合成和性质研究
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摘要
本论文主要采用溶剂热(水热)法合成了一系列新颖的配位聚合物,并用元素分析、红外光谱和单晶衍射等分析手段进行了表征。这些聚合物分别是:[Mn(ndc)(bpy)·H_2O] (1)、[Mn(ndc)(phen)] (2)、[Mn_3(ndc)_3(bpy)_2] (3)、[Cu_2(pz)_3(ClO_4)_2] (4)、[Cu(pz)_2(ClO_4)·3H_2O] (5)、[Zn(ndc)(pn)_2] (6)。对部分化合物还进一步进行了不同温度下的摩尔磁导率测试。论文内容包括如下:
1.以过渡金属锰盐和有机配体2,6-萘二酸(ndc)及2,2'-联吡啶(bpy)和1,10-菲啰啉(phen)进行反应,用溶剂热方法合成了三个3D结构的锰配位聚合物。测试了这些聚合物在不同温度下的摩尔磁矩,结果显示配位聚合物(1)和(2)是反铁磁性,配位聚合物(3)为铁磁性。
2.通过单晶结构分析和元素分析,描述了两个新的以铜(Ⅰ)作为中心金属,吡嗪为桥联配体的配位聚合物的合成方法及结构特征。配位聚合物(4)是以三配位六元环状铜(Ⅰ)为特征的2D晶体结构,而配位聚合物(5)是以四配位铜(Ⅰ)为特征的3D网状晶体结构。两者的结构与已报道的类似结构化合物进行了比较。并探讨了合成条件对配位聚合物结构的影响。
3.用高氯酸锌和2,6-萘二酸(ndc)及丙二胺(pn)作为反应物,通过溶剂热方法合成了一个一维链状结构的配位聚合物(6)。通过与文献报道的相关配位聚合物结构的比较,探讨了配体在结构组装上的作用。
In this thesis, a series of novel coordination polymers were synthesized by solvothermal/hydrothermal method and characterized by elemental analysis,IR spectroscopy and single-crystal X-ray diffraction. These compounds are as followed [Mn(ndc)(bpy)-H_2O] (1),[Mn(ndc)(phen)] (2), [Mn_3(ndc)_3(bpy)_2] (3), [Cu_2(pz)_3(C1O_4)2] (4),[Cu(pz)_2(C1O_4)·3H_2O] (5) and [Zn(ndc)(pn)_2] (6) respectively. And part of the compounds have been further characterized by variable-temperature magnetic susceptibility measurements. This thesis is consist of the following contents:
1. Three novel 3D metal-organic coordination polymers were hydrothermal synthesized via the reaction between manganese salt and organic lignads ndc, bpy and phen. The magnetic properties of the three compounds were investigated by variable-temperature magnetic susceptibility, and the results reveal that compound (1) and (2) are of antiferromagnetic property, while compound (3) is of ferromagnetic property.
2. We describe the preparation and the structural characteristics of two novel copper(Ⅰ)-pz coordination polymers by single-crystal X-ray diffraction and element analysis. Compound (4) is a 2D net structural crystal with 3-coordinated Cu(Ⅰ); Compound (5) is a 3D framework crystal with 4-coordinated Cu(Ⅰ).They are compared with other reported similar structures.
3. A 1D coordination polymer was synthesized by the reaction of Zn(ClO_4)_2 with ndc and pn.Comparing to the related compounds, the role of the ligands in the formation of the compound (6) was discussed.
1.以过渡金属锰盐和有机配体2,6-萘二酸(ndc)及2,2'-联吡啶(bpy)和1,10-菲啰啉(phen)进行反应,用溶剂热方法合成了三个3D结构的锰配位聚合物。测试了这些聚合物在不同温度下的摩尔磁矩,结果显示配位聚合物(1)和(2)是反铁磁性,配位聚合物(3)为铁磁性。
2.通过单晶结构分析和元素分析,描述了两个新的以铜(Ⅰ)作为中心金属,吡嗪为桥联配体的配位聚合物的合成方法及结构特征。配位聚合物(4)是以三配位六元环状铜(Ⅰ)为特征的2D晶体结构,而配位聚合物(5)是以四配位铜(Ⅰ)为特征的3D网状晶体结构。两者的结构与已报道的类似结构化合物进行了比较。并探讨了合成条件对配位聚合物结构的影响。
3.用高氯酸锌和2,6-萘二酸(ndc)及丙二胺(pn)作为反应物,通过溶剂热方法合成了一个一维链状结构的配位聚合物(6)。通过与文献报道的相关配位聚合物结构的比较,探讨了配体在结构组装上的作用。
In this thesis, a series of novel coordination polymers were synthesized by solvothermal/hydrothermal method and characterized by elemental analysis,IR spectroscopy and single-crystal X-ray diffraction. These compounds are as followed [Mn(ndc)(bpy)-H_2O] (1),[Mn(ndc)(phen)] (2), [Mn_3(ndc)_3(bpy)_2] (3), [Cu_2(pz)_3(C1O_4)2] (4),[Cu(pz)_2(C1O_4)·3H_2O] (5) and [Zn(ndc)(pn)_2] (6) respectively. And part of the compounds have been further characterized by variable-temperature magnetic susceptibility measurements. This thesis is consist of the following contents:
1. Three novel 3D metal-organic coordination polymers were hydrothermal synthesized via the reaction between manganese salt and organic lignads ndc, bpy and phen. The magnetic properties of the three compounds were investigated by variable-temperature magnetic susceptibility, and the results reveal that compound (1) and (2) are of antiferromagnetic property, while compound (3) is of ferromagnetic property.
2. We describe the preparation and the structural characteristics of two novel copper(Ⅰ)-pz coordination polymers by single-crystal X-ray diffraction and element analysis. Compound (4) is a 2D net structural crystal with 3-coordinated Cu(Ⅰ); Compound (5) is a 3D framework crystal with 4-coordinated Cu(Ⅰ).They are compared with other reported similar structures.
3. A 1D coordination polymer was synthesized by the reaction of Zn(ClO_4)_2 with ndc and pn.Comparing to the related compounds, the role of the ligands in the formation of the compound (6) was discussed.
引文
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