1，8-萘二甲酸配位聚合物的水热合成、晶体结构及性能研究
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摘要
金属-有机配位聚合物的合成和性质研究成为化学和材料科学的活跃的研究领域之一,而有机配体的选择无疑是重要的。芳香羧酸配体因具有好的结构刚性和热稳定性被广泛应用于配合物的构筑。在本论文中我们选择1,8-萘二酸酐作为初始配体,理由如下:1,8-萘二酸酐在水热条件下水解成为1,8-萘二甲酸。1,8-萘二甲酸有两个羧基和一个芳香环,存在丰富的配位模式,可以构筑新颖的结构。氢键作用和π-π相互作用的存在可以稳定配合物或者构筑超分子配合物。通过1,8-萘二甲酸构筑的金属-有机配位聚合物有9个:
1.[Zn(1,8-nap)(H_2O)]_n(1)
2.[Zn4(1,8-nap)_4(4,4'-bipy)_2·0.5en·H_2O]_n(2)
3.[Cd(1,8-nap)]_n(3)
4.{[Cd_2(1,8-nap)_2(H_2O)_2](bpp)_2}_n(4)
5.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(5)
6.[Mn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·4H_2O(6)
7.[Zn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_4]·2H_2O(7)
8.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(8)
9.[Zn_2(1,8-nap)_2(2,2'-bipy)_2(H_2O)_2]·4H_2O(9)单晶X-射线衍射研究发现:配合物1是一个二维层状结构,配合物2是一个一维双链,配合物3是一个6连接的(3,6)网状拓扑结构,配合物4是同时含有16原子环和24原子环的一维链,配合物5、6、8、9是由氢键和π-π相互作用构筑的三维超分子网络,配合物5和8的羧酸配位模式不同,配合物7是由两种π-π相互作用构筑的二维层状结构。对配合物进行红外、元素分析、热稳定性以及荧光等方面的研究。
The synthesis and property of metal-organic hybrid complexes have represented one of the most active research areas in chemistry and materials science. The selection of the appropriate organic ligand is the most important key in the research areas. Aromatic carboxylic acids, which possess good structure rigidity and thermo-stability, have broadly been used in the construction of new complexes. In this thesis, we select naphthalene-1,8-dicarboxylic anhydride as our origin ligand. The reason is as follows: Naphthalene-1,8-dicarboxylic anhydride can hydrolyze under hydrothermal conditions into the naphthalene-1,8-dicarboxylate ligand. Naphthalene-1,8-dicarboxylate ligand has two carboxyl groups and a naphthalene ring, including rich coordination modes, so we can use naphthalene-1,8-dicarboxylate as links to build novel structures. Hydrogen bonds andπ-πinteractions can consolidate complexes or build supramolecular structures. We have hydrothermally synthesized nine metal-organic complexes with naphthalene-1, 8-dicarboxylate:
1.[Zn(1,8-nap)(H_2O)]_n(1)
2.[Zn4(1,8-nap)_4(4,4'-bipy)_2·0.5en·H_2O]_n(2)
3.[Cd(1,8-nap)]_n(3)
4.{[Cd_2(1,8-nap)_2(H_2O)_2](bpp)_2}_n(4)
5.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(5)
6.[Mn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·4H_2O(6)
7.[Zn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_4]·2H_2O(7)
8.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(8)
9.[Zn_2(1,8-nap)_2(2,2'-bipy)_2(H_2O)_2]·4H_2O(9)
The results of the X-ray single-crystal structure analysis are as follows: Complex 1 is a two-dimensional layer. Complex 2 is a one-dimensional double chain. Complex 3 is a six-connected (3, 6) network topology structure. Complex 4 is a one-dimensional chain with one 16-membered ring and one 24-membered ring. Complexes 5、6、8、9 are three-dimensional supramolecular networks constructed by hydrogen bonds andπ-πinteractions. The coordination modes of carboxylate in complex 5 and complex 8 are different. Complex 7 is a two-dimensional layer constructed by two kinds ofπ-πinteractions. We have studied the IR, elementary analysis, thermo-gravimetric property and luminescence property.
1.[Zn(1,8-nap)(H_2O)]_n(1)
2.[Zn4(1,8-nap)_4(4,4'-bipy)_2·0.5en·H_2O]_n(2)
3.[Cd(1,8-nap)]_n(3)
4.{[Cd_2(1,8-nap)_2(H_2O)_2](bpp)_2}_n(4)
5.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(5)
6.[Mn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·4H_2O(6)
7.[Zn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_4]·2H_2O(7)
8.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(8)
9.[Zn_2(1,8-nap)_2(2,2'-bipy)_2(H_2O)_2]·4H_2O(9)单晶X-射线衍射研究发现:配合物1是一个二维层状结构,配合物2是一个一维双链,配合物3是一个6连接的(3,6)网状拓扑结构,配合物4是同时含有16原子环和24原子环的一维链,配合物5、6、8、9是由氢键和π-π相互作用构筑的三维超分子网络,配合物5和8的羧酸配位模式不同,配合物7是由两种π-π相互作用构筑的二维层状结构。对配合物进行红外、元素分析、热稳定性以及荧光等方面的研究。
The synthesis and property of metal-organic hybrid complexes have represented one of the most active research areas in chemistry and materials science. The selection of the appropriate organic ligand is the most important key in the research areas. Aromatic carboxylic acids, which possess good structure rigidity and thermo-stability, have broadly been used in the construction of new complexes. In this thesis, we select naphthalene-1,8-dicarboxylic anhydride as our origin ligand. The reason is as follows: Naphthalene-1,8-dicarboxylic anhydride can hydrolyze under hydrothermal conditions into the naphthalene-1,8-dicarboxylate ligand. Naphthalene-1,8-dicarboxylate ligand has two carboxyl groups and a naphthalene ring, including rich coordination modes, so we can use naphthalene-1,8-dicarboxylate as links to build novel structures. Hydrogen bonds andπ-πinteractions can consolidate complexes or build supramolecular structures. We have hydrothermally synthesized nine metal-organic complexes with naphthalene-1, 8-dicarboxylate:
1.[Zn(1,8-nap)(H_2O)]_n(1)
2.[Zn4(1,8-nap)_4(4,4'-bipy)_2·0.5en·H_2O]_n(2)
3.[Cd(1,8-nap)]_n(3)
4.{[Cd_2(1,8-nap)_2(H_2O)_2](bpp)_2}_n(4)
5.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(5)
6.[Mn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·4H_2O(6)
7.[Zn_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_4]·2H_2O(7)
8.[Cd_4(1,8-nap)_4(2,2'-bipy)_4(H_2O)_8]·6H_2O(8)
9.[Zn_2(1,8-nap)_2(2,2'-bipy)_2(H_2O)_2]·4H_2O(9)
The results of the X-ray single-crystal structure analysis are as follows: Complex 1 is a two-dimensional layer. Complex 2 is a one-dimensional double chain. Complex 3 is a six-connected (3, 6) network topology structure. Complex 4 is a one-dimensional chain with one 16-membered ring and one 24-membered ring. Complexes 5、6、8、9 are three-dimensional supramolecular networks constructed by hydrogen bonds andπ-πinteractions. The coordination modes of carboxylate in complex 5 and complex 8 are different. Complex 7 is a two-dimensional layer constructed by two kinds ofπ-πinteractions. We have studied the IR, elementary analysis, thermo-gravimetric property and luminescence property.
引文
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