含四唑配子之銅配位聚合物之自組裝合成、結構鑑定與性質研究

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Title:	含四唑配子之銅配位聚合物之自組裝合成、結構鑑定與性質研究 Self-assembly, Structures and Properties of Copper-Containing Coordination Polymers Based on Tetrazole Ligand
Authors:	唐偉仁 Tang, Wei-Ren
Contributors:	化學系應用化學碩士班
Keywords:	自組裝配位聚合物銅離子 tetrazole配位子 self-assembly coordination polymers copper tetrazole
Date:	2013-06
Issue Date:	2013-10-08 14:49:44 (UTC+8)
Abstract:	四唑配子為一個五員環含有四個氮原子的雜環官能基，這個官能基具有四個氮的配位點，故與金屬離子配位時可能具有相當大的多變性。本論文探討含有tetrazole官能基的5-(4-pyridyl)tetrazole (4-Hptz) 配子與銅金屬離子之水熱自組裝反應，並研究生成的配位聚合物結構與各項性質。醋酸銅與4-H-ptz及稀釋的磷酸進行水熱自組裝合成，得到二維的配位聚合物{[Cu(4-ptz)2(H2O)2] }n (1)；利用4-Hptz和1,5-naphtalenedisulfonate(1,5-Na2nds)與硝酸銅進行水熱自組裝合成，得到配位聚合物2－4，分別為二維{[Cu(OH)(1,5nds)0.5(4-ptz)]•H2O}n (2)、三維{[Cu3(OH)(1,5nds)(4-ptz)3 (H2O)4]•toluene}n (3)與一維{[Cu(1,5nds)(4-ptz)2(H2O)2]•2H2O}n (4)；4-H-ptz和sodium 3,5-dicarboxybenzenesulfonate (NaH2sip)與氯化銅進行水熱自組裝合成，得到配位聚合物{[Cu2(NaHsip)2(4-ptz)2(H2O)4]•2H2O}n (5)，若與硝酸銅進行水浴自組裝合成，得到{[Cu3(OH)3(4-ptz)3(H2O)4]•4H2O}n (6). 本論文中共合成出6個銅金屬-有機配位聚合物，其結構經紅外線吸收光譜、元素分析及單晶、粉末X-ray繞射解析鑑定，並利用熱重分析儀測定其熱穩定性質。 Tetrazole possesses a five-membered heterocyclic group that contains for N donors. The goal of this study was to develop a self-assembly synthetic strategy for the preparation of coordination polymers using the tetrazolate ligand 5-(4-pyridyl)tetrazole (4-Hptz). The synthetic method, the structures of the products were investigated. The reaction of Cu(CH3COO)2•H2O with 4-Hptz and H3PO4(aq) under hydrothermal conditions produced a 2D coordination polymer {[Cu(4-ptz)2(H2O)2]}n (1). The reaction of Cu(NO3)2•3H2O with 4-H-ptz and 1,5-naphtalenedisulfonate (1,5-Na2nds) under hydrothermal conditions afforded a 2D coordination polymer {[Cu(OH)(1,5nds)0.5(4-ptz)]•H3O}n (2), a 3D coordination polymer {[Cu3(OH)(1,5nds) (4-ptz)3(H2O)4]•toluene}n (3), and a 1D coordination polymer {[Cu(1,5nds)(4-ptz)2 (H2O)2] •2H3O•2H2O}n (4). The reaction of CuCl2•2H2O with 4-Hptz and sodium 3,5-dicarboxybenzenesulfonate (NaH2sip) under hydrothermal conditions afforded a monomeric molecule {[Cu2(NaHsip)2(4-ptz)2(H2O)4]•2H2O}n (5), and reaction of Cu(NO3)2•3H2O under water bath conditions resulted in the formation of a 3D coordination polymer {[Cu3(OH)3(4-ptz)3(H2O)4]•4H2O}n (6). The structures of the six coordination polymers were characterized by IR spectroscopy, elemental analysis and single-crystal or powder X-ray diffraction methods. The thermal stability and photophysical properties of the products were evaluated by TGA and solid state emission spectroscopy.
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