氮杂环羧酸—过渡金属配合物的合成与结构及性质研究
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摘要
本文主要通过吡嗪二甲酸、含氮杂环的功能性设计,研究了这类配体与过渡金属配合物的结构,共得到了10个吡嗪二甲酸、含氮杂环和过渡金属的配合物,通过对配合物结构与性质的研究,为功能配合物的设计合成提供了一些新的方法和思路。本文共分3章。
第1章介绍了配位化学的进展,超分子配位聚合物的概念和应用,重点介绍含氮羧酸、含氮杂环配合物的研究现状,同时对本论文选题意义做了概述。
第2章介绍了以2,3-吡嗪二甲酸为配体,选择不同的含氮杂环进行混配,与CdSO_4、CoSO_4、MnSO_4、CuI等金属盐在溶剂热的条件下反应,得到五个配合物,通过X-射线单晶衍射确定了它们的结构。配合物[Cd(Trz)_3(pzdc)_2]n(1)和配合物[Co(Trz)(2-pzdc)_2]n(2)是三维的结构。配合物[Mn(μ2-2,3-pzdc)phen]n(3)]n配合物[Cd(μ2-2,3-pzdc)(2,2-bpy)]n(4)由于配体间的氢键和π-π堆积作用,从二维形成三维结构。配合物Cu(2,3-pzdc)_2(H_2O)_2(5)是单核结构。
第3章先介绍了用CdSO_4分别与三氮唑、氨基四氮唑通过溶剂热法合成出的三个配合物[Cd_2(Ata)SO_4·OH]n(6),[Cd_5(Ata)_4(SO_4)_2(OH)_2]n(7)和[Cd_2(Trz)(SO_4)(OH)]n(8),三个配合物都是三维结构,其中配合物6和配合物7,由于合成条件pH值的不同,配合物6中Cd有两种不同配位模式,而在配合物7中Cd有三种不同配位模式。接着介绍用2,2-联吡啶与铜盐合成的两个配合物[Cu(2-bpy)_2 I_2](9)、[Cu(2-bpy)_2(NO_3)_2·H_2O](10)。两个是单核的结构,结构中都存在氢键和π-π堆积作用,其中配合物X中有一个游离的NO_3和游离的H_2O,在结构中存在annion-π的堆积作用。
The rational design and research of structures and special functions represent one of the rapidly developing fields in current coordination and supramolecular chemistry.This thesis focuses on the design and syntheses of transitional-metal complexes by 2,3-pyrazinedicarboxylic acid and nitrogen heterocycle.The crystal structures of the complexes were determined by single-crystal X-ray diffraction and IR spectrometry.This work provides some new methods and thoughts in the design and synthesis of heterometallic terpyridine complexes.
The thesis is divided into three chapters.
In the first chapter,the concept,history and application of coordination chemistry and supramolecular complexes are concisely introduced.The background of this work is also briefly reviewed with the emphasis on nitrogen carboxylic and nitrogen heterocycle.In addition,the significancy of this work was also described.
In the second chapter,the reactions of ligand 2,3-pyrazinedicarboxylic acid and nitrogen heterocycle with transitional-metal under solvothermal conditions have been carried out.Five novel complexes.Complex 1 and Complex 2 are 3D polymer.Complex 3 and Complex 4 are 3D polymer formed by hydrogening bond andπ-πpacking.Complex 5 is a 1D polymer.
The third chapter focuses on three complexes,synthesize with CdSO_4 and 1,2,4-Triazole or 5-Amino Tetrazole.They are 3D.Complex 6,7 and 8 are different on structure of influences of pH in synthesize.There are two complex type of Cd in complexes 6,three complex type of Cd in complexes 7.Two complexes are synthesize with CuSO_4 and 2,2-Bipyridine.There are by hydrogening bond,π-πand annion-πpacking in complexes.
第1章介绍了配位化学的进展,超分子配位聚合物的概念和应用,重点介绍含氮羧酸、含氮杂环配合物的研究现状,同时对本论文选题意义做了概述。
第2章介绍了以2,3-吡嗪二甲酸为配体,选择不同的含氮杂环进行混配,与CdSO_4、CoSO_4、MnSO_4、CuI等金属盐在溶剂热的条件下反应,得到五个配合物,通过X-射线单晶衍射确定了它们的结构。配合物[Cd(Trz)_3(pzdc)_2]n(1)和配合物[Co(Trz)(2-pzdc)_2]n(2)是三维的结构。配合物[Mn(μ2-2,3-pzdc)phen]n(3)]n配合物[Cd(μ2-2,3-pzdc)(2,2-bpy)]n(4)由于配体间的氢键和π-π堆积作用,从二维形成三维结构。配合物Cu(2,3-pzdc)_2(H_2O)_2(5)是单核结构。
第3章先介绍了用CdSO_4分别与三氮唑、氨基四氮唑通过溶剂热法合成出的三个配合物[Cd_2(Ata)SO_4·OH]n(6),[Cd_5(Ata)_4(SO_4)_2(OH)_2]n(7)和[Cd_2(Trz)(SO_4)(OH)]n(8),三个配合物都是三维结构,其中配合物6和配合物7,由于合成条件pH值的不同,配合物6中Cd有两种不同配位模式,而在配合物7中Cd有三种不同配位模式。接着介绍用2,2-联吡啶与铜盐合成的两个配合物[Cu(2-bpy)_2 I_2](9)、[Cu(2-bpy)_2(NO_3)_2·H_2O](10)。两个是单核的结构,结构中都存在氢键和π-π堆积作用,其中配合物X中有一个游离的NO_3和游离的H_2O,在结构中存在annion-π的堆积作用。
The rational design and research of structures and special functions represent one of the rapidly developing fields in current coordination and supramolecular chemistry.This thesis focuses on the design and syntheses of transitional-metal complexes by 2,3-pyrazinedicarboxylic acid and nitrogen heterocycle.The crystal structures of the complexes were determined by single-crystal X-ray diffraction and IR spectrometry.This work provides some new methods and thoughts in the design and synthesis of heterometallic terpyridine complexes.
The thesis is divided into three chapters.
In the first chapter,the concept,history and application of coordination chemistry and supramolecular complexes are concisely introduced.The background of this work is also briefly reviewed with the emphasis on nitrogen carboxylic and nitrogen heterocycle.In addition,the significancy of this work was also described.
In the second chapter,the reactions of ligand 2,3-pyrazinedicarboxylic acid and nitrogen heterocycle with transitional-metal under solvothermal conditions have been carried out.Five novel complexes.Complex 1 and Complex 2 are 3D polymer.Complex 3 and Complex 4 are 3D polymer formed by hydrogening bond andπ-πpacking.Complex 5 is a 1D polymer.
The third chapter focuses on three complexes,synthesize with CdSO_4 and 1,2,4-Triazole or 5-Amino Tetrazole.They are 3D.Complex 6,7 and 8 are different on structure of influences of pH in synthesize.There are two complex type of Cd in complexes 6,three complex type of Cd in complexes 7.Two complexes are synthesize with CuSO_4 and 2,2-Bipyridine.There are by hydrogening bond,π-πand annion-πpacking in complexes.
引文
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