【摘要】：配位聚合物(coordination polymers,CPs),也稱金屬有機(jī)骨架(Metal organic frameworks,MOFs),作為化學(xué)和材料科學(xué)中最受關(guān)注的研究領(lǐng)域之一,近年來展現(xiàn)出非常迅速的發(fā)展趨勢(shì),并成為多孔材料家族中一個(gè)重要的組成部分。CPs不僅具有豐富的拓?fù)浣Y(jié)構(gòu),而且在許多領(lǐng)域具有潛在的應(yīng)用價(jià)值,例如氣體吸附和分離、催化、發(fā)光、感測(cè)和質(zhì)子傳導(dǎo)等。它們的結(jié)晶特性、高孔隙率、均勻分布的孔徑、大的表面積、可調(diào)控的孔表面特性以及潛在的工業(yè)規(guī)模的可擴(kuò)展性使得這類材料有著進(jìn)一步研究的潛能。在諸多配位聚合物的類型中,以稀土離子作為金屬中心的一類受到人們廣泛的關(guān)注。由于稀土離子通常采用八配位或者十二配位的配位模式,并且具有特殊的發(fā)光特性,使其構(gòu)筑的配位聚合物具有多樣的結(jié)構(gòu)和優(yōu)良的光學(xué)特性。此外,在有機(jī)配體中引入雜原子如N原子,大大提高了新穎結(jié)構(gòu)的配位聚合物生成的可能。本論文選用含N雙羧酸配體作為有機(jī)配體,金屬鈧以及銪、鋱、釓、鉺等鑭系金屬作為金屬中心,在水熱及溶劑熱的條件下,合成出六個(gè)配位聚合物,對(duì)這六個(gè)配位聚合物的發(fā)光、催化以及吸附性能進(jìn)行了研究。主要工作內(nèi)容如下:1、分別以2,5-吡啶二羧酸(2,5-pyridinedicarboxylic acid,H_2L~1)、2,3-吡嗪二羧酸(2,3-pyrazinedicarboxylic acid,H_2L~2)為有機(jī)配體,金屬鈧為金屬中心,合成了兩個(gè)配位聚合物[Sc_2L_2~1(HL~1)_2(H_2O)_2]·H_2O(1)和ScL~2(HL~2)(DMF)(2)�；衔�1為2D層狀結(jié)構(gòu),化合物2為1D鏈狀結(jié)構(gòu)�；衔�1表現(xiàn)出良好的熒光性能和染料吸附性能,此外還有良好的催化性能�；衔�2表現(xiàn)出良好的催化性能和熒光性能。(見第二章)2、以鑭系元素銪、鋱、釓、鉺為金屬源,分別以2,5-吡嗪二羧酸(2,5-pyrazinedicarboxylic acid,H_2L~3)、2,5-吡啶二羧酸(2,5-pyridinedicarboxylic acid,H_2L~1)為有機(jī)配體,合成了四個(gè)配位聚合物Na[Eu(C_2O_4)_2(H_2O)]·2H_2O(3)、Na[Tb(C_2O_4)_2(H_2O)]·2H_2O(4)、Na[Gd(C_2O_4)_2(H_2O)]·2H_2O(5)和Er_4L_4~1(DMF)(OH)_4(H_2O)(6)�；衔�3-5是同構(gòu)的,合成過程中有機(jī)溶劑發(fā)生了原位反應(yīng),形成了2D層狀結(jié)構(gòu)�；衔�6是具有四核簇的3D結(jié)構(gòu)。我們對(duì)化合物3-5進(jìn)行了熒光測(cè)試,它們表現(xiàn)出相應(yīng)鑭系金屬離子的特征發(fā)射光譜,此外還對(duì)化合物3進(jìn)行了染料吸附測(cè)試,發(fā)現(xiàn)其有一定的染料吸附能力。對(duì)于化合物6,我們進(jìn)行了近紅外區(qū)的熒光測(cè)試,其表現(xiàn)出金屬中心鉺的特征峰,并且化合物6還有著良好的染料吸附性能。
[Abstract]:Coordination polymer (coordination polymers,CPs), also known as metal organic skeleton (Metal organic frameworks,MOFs), as one of the most concerned research fields in chemistry and material science, has shown a very rapid development trend in recent years. CPs not only has rich topological structure, but also has potential application value in many fields, such as gas adsorption and separation, catalysis, luminous, sensing and proton conduction. Their crystallization characteristics, high porosity, uniform pore size, large surface area, adjustable pore surface characteristics and potential industrial scale scalability make this kind of materials have the potential for further research. Among many types of coordination polymers, rare earth ions as metal centers have attracted extensive attention. Because rare earth ions usually adopt eight or twelve coordination modes and have special luminous properties, the coordination polymers constructed by rare earth ions have various structures and excellent optical properties. In addition, the introduction of hetero atoms such as N atoms into organic ligands greatly improves the possibility of the formation of coordination polymers with novel structures. In this paper, six coordination polymers were synthesized by using N-dicarboxylic acid ligands as organic ligands, Scandium metal and lanthanide metals such as europium, terbium, gadolinium and erbium as metal centers under hydrothermal and solvothermal conditions. The luminous, catalytic and adsorption properties of the six coordination polymers were studied. The main contents are as follows: 1) 2,5-pyridyl dicarboxylic acid (2,5 pyridinedicarboxylic acid,H_2L~1), 2, 3-pyrazide dicarboxylic acid (2, 3 pyrazinedicarboxylic acid,H_2L~2) were used as organic ligands and SC as metal center, respectively. Two coordination polymers [Sc_2L_2~1 (HL~1) _ 2 (H 鈮，

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