芳香二酸基d~（10）金属配合材料的构筑及其降解酸性品红性能研究
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摘要
利用分子组装原理精心设计和调控高级有序结构分子聚集体,尤其是配位聚合物或超分子聚合物是当今化学、材料、医学和生物学等领域的前沿研究主流和热点课题。由于配合物分子固体同时含有无机金属和有机配体,使其在材料设计和功能复合上具有区别于纯无机或纯有机固体的优势和发展空间。目前文献报道的功能配合材料主要集中在磁性、光学、电学和生物等功能方面,而对其催化性能的研究报道较少。本文以邻、间、对苯二乙酸为基本构件,过渡金属离子Zn、Cd为中心离子,并辅以芳香族含N配体,构筑了12个新型有机-无机功能配合材料,它们是:{[Cd(1,4-pda)(bpb)(H_2O)]·H_2O}_n (1),{[Zn2(1,3-pda)_2(phen)_2]·4H_2O}_n(2),{[Cd_2(1,3-pda)_2(bpy)_2]·2H_2O}_n(3) , {[Cd_2(1,3-pda)(phen)]·2H_2O}_n(4) ,[Zn(1,3-pda)(bpp)]_n(5) , {[Zn(1,2-pda)(phen)_4]·NO_3·4H_2O}_n(6) ,[Zn(1,2-Hpda)_2(bpy)]_n(7) , [Zn(1,2-pda)_2(bpy)(H_2O)]_n(8) ,{[Cd_2(1,2-pda)_2(phen)_3(H_2O)]·EtOH·3H_2O}_n (9)、[Cd_2(1,2-pda)_2(bpy)_2(H_2O)_2]_n(10) ,{[Cd_2(1,2-pda)_2(ip)4]·3H_2O}_n(11),[Cd_2(1,2-pda)_2(ip)4]_n(12);对所合成的配合材料进行了单晶结构测试和分析,运用红外光谱、荧光光谱、热分析等技术对其进行了表征;最后以酸性品红为模型污染物,考察了配合物及其敏化纳米TiO_2的光催化降解性能。结果表明,上述三类配体在功能分子材料的构筑中起到了重要作用,它们不仅呈现出多种配位方式,而且可作为氢键的给-受体形成高维扩展结构,同时对三种苯二乙酸构筑的功能配合材料的结构特点、组装规律、谱学特征、荧光性质、光催化降解及其敏化TiO_2的光催化性能进行了比较分析,得出了一些规律性结论。
The exquisite designed construction of metal-assembled and metal-cluster frameworks by use of the principles of self-assembly, especially for coordination polymers and supramolecular architectures, represents a topical and current research interest in chemistry, materials, medicals and biology areas today. As complexe molecular solid contain inorganic metal and organic ligand at the same time, so it has more advantage and developmental space in the facet of material design and functional complex, which is compared with pure inorganic and organic solid. Presently, literatures about functional complex materials mostly focus on magnetism, optics, electricity, biology, but the report about its catalytic area is still rare. In this theses, we choose O-Phenylenediacetic acid(1,2-H_2pda)、m-Phenylenediacetic acid(1,3-H_2pda)、p-Phenylenediacetic acid(1,4-H_2pda), as building units and use transition metal ions as Zn, Cd metal center, meanwhile, accompany aromatic ligands including N donors. As results, 12 novel organo-matel supramolecular polymers namely {[Cd(1,4-pda)(bpb)(H_2O)]·H_2O}_n(1) , {[Zn2(1,3-pda)_2(phen)_2]·4H_2O}_n(2) ,{[Cd_2(1,3-pda)_2(bpy)_2]·2H_2O}_n(3) , {[Cd_2(1,3-pda)(phen)]·2H_2O}_n(4) ,[Zn(1,3-pda)(bpp)]_n(5) , {[Zn(1,2-pda)(phen)4]·NO3·4H_2O}_n(6) ,[Zn(1,2-Hpda)_2(bpy)]_n(7) , [Zn(1,2-pda)_2(bpy)(H_2O)]_n(8) ,{[Cd_2(1,2-pda)_2(phen)_3(H_2O)]·EtOH·3H_2O}_n (9)、[Cd_2(1,2-pda)_2(bpy)_2(H_2O)_2]_n(10) ,{[Cd_2(1,2-pda)_2(ip)4]·3H_2O}_n(11),[Cd_2(1,2-pda)_2(ip)4]_n(12);The 12 complexes have been determined by the X-ray single crystal diffraction analysis, and IR spectra, thermal analyses were used to investigate their spectroscopy characters and properties. Finally, Nanoporous TiO_2 sensitized by complex has been used for cheaking photocatalytic activity for degradation of acidic fuchsin as stimulant dyes. The results show that the 3 kinds of phenylenediacetic acids mentioned above play an important role in the construction of novel organo-metal supramolecular polymers, which could act as donor-acceptor of hydrogen bonds formulating multi-dimensional expanded networks. Meanwhile, some regular conclusion have been summarized through the comparison studies on structures, assembled rules, spectroscopy characters, fluorescence,photocatalytic activity of TiO_2 sensitized by compounds of the supramolecular polymers constructed from 3 kinds of phenylenediacetic acids.
The exquisite designed construction of metal-assembled and metal-cluster frameworks by use of the principles of self-assembly, especially for coordination polymers and supramolecular architectures, represents a topical and current research interest in chemistry, materials, medicals and biology areas today. As complexe molecular solid contain inorganic metal and organic ligand at the same time, so it has more advantage and developmental space in the facet of material design and functional complex, which is compared with pure inorganic and organic solid. Presently, literatures about functional complex materials mostly focus on magnetism, optics, electricity, biology, but the report about its catalytic area is still rare. In this theses, we choose O-Phenylenediacetic acid(1,2-H_2pda)、m-Phenylenediacetic acid(1,3-H_2pda)、p-Phenylenediacetic acid(1,4-H_2pda), as building units and use transition metal ions as Zn, Cd metal center, meanwhile, accompany aromatic ligands including N donors. As results, 12 novel organo-matel supramolecular polymers namely {[Cd(1,4-pda)(bpb)(H_2O)]·H_2O}_n(1) , {[Zn2(1,3-pda)_2(phen)_2]·4H_2O}_n(2) ,{[Cd_2(1,3-pda)_2(bpy)_2]·2H_2O}_n(3) , {[Cd_2(1,3-pda)(phen)]·2H_2O}_n(4) ,[Zn(1,3-pda)(bpp)]_n(5) , {[Zn(1,2-pda)(phen)4]·NO3·4H_2O}_n(6) ,[Zn(1,2-Hpda)_2(bpy)]_n(7) , [Zn(1,2-pda)_2(bpy)(H_2O)]_n(8) ,{[Cd_2(1,2-pda)_2(phen)_3(H_2O)]·EtOH·3H_2O}_n (9)、[Cd_2(1,2-pda)_2(bpy)_2(H_2O)_2]_n(10) ,{[Cd_2(1,2-pda)_2(ip)4]·3H_2O}_n(11),[Cd_2(1,2-pda)_2(ip)4]_n(12);The 12 complexes have been determined by the X-ray single crystal diffraction analysis, and IR spectra, thermal analyses were used to investigate their spectroscopy characters and properties. Finally, Nanoporous TiO_2 sensitized by complex has been used for cheaking photocatalytic activity for degradation of acidic fuchsin as stimulant dyes. The results show that the 3 kinds of phenylenediacetic acids mentioned above play an important role in the construction of novel organo-metal supramolecular polymers, which could act as donor-acceptor of hydrogen bonds formulating multi-dimensional expanded networks. Meanwhile, some regular conclusion have been summarized through the comparison studies on structures, assembled rules, spectroscopy characters, fluorescence,photocatalytic activity of TiO_2 sensitized by compounds of the supramolecular polymers constructed from 3 kinds of phenylenediacetic acids.
引文
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