mn-mofs及nimil-120的合成及其催化性能的研究

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'mn-mofs及nimil-120的合成及其催化性能的研究'
金属-有机骨架化合物(Metal-Organic Frameworks, MOFs)是由无机金屈离 子和有机配体配位而成的一类新型晶体材料,近年来因其独特性质而受到广泛 关注。MOFs材料具有空隙率高(可高达90%的孔体积)、内比表面大(高达 6000 m2/g)、结构可调控以及金属离了和表面有机官能团多样等特:点,在清洁 能源、气体存储与分离、生物医学成像、薄层技术以及催化等方而具有巨大的 潜在应用。MOFs材料在催化中的应用可以分为金属离子活性位点催化(Open Metal Sites, OMS),功能化有机配体催化(Functional Organic Sites, FOS)以及 作为载体三种。本课题针对其中第一种OMS催化形式,利用有机配体N, N\ N" -三(4-苯甲酸基)-1, 3, 5-苯三甲酰胺和乙酸镭合成MOFS晶体并将其应用 于脑文格反应。针对第三种催化形式,利用MIL-120负载镰作为活性组分来催 化苯述原反应。1. ^(CH3COO)2Mn-4H2O 和 N, N\ N" -三(4—苯甲酸基)一1, 3, 5-苯三甲酰 胺(H3L)在水热条件下,以2, T -联毗睫(bpy)作为第二配体合成了一个一 维晶体[Mn(L)(bpy)] (1),以1,仁(1,4?丁基)二咪卩坐(bbi)作为第二配体合成了另 一二维晶体[Mn(L)0.5(bbi)2.5(H2O)] (2),将两个晶体应用催化于knoevenagel反 应。实验表明,化合物1具有一维结构能够更加充分地和反应物进行接触,有 利于反应进行,因此晶体1比2具有更好的催化效果。2. 在水热条件下,利用均苯四甲酸和硝酸铝自组装合成具有高热稳定的 MIL-120,并将其作为载体通过浸渍法负载镰得到还原催化剂x-NM,把该还原 催化剂应用到苯还原反应。实验表明,负载量为15%的15-NM具有最好的催化 活性。关键词:MOFs; Mm催化;脑文格反应;苯述原反应ABSTRACTMetal-organic frameworks (MOFs),a series of new crystalline and porous solid materials constructed from inorganic metal-ion clusters and polytopic organic linkers, are receiving significant attention recently? MOFs possess ultrahigh porosity (up to 90% fi*ee volume), large internal surface area (up to 6000 m2/g), adjustable structure, and variability of the functionality of metal ions and organic ligands, thus MOFs show great potential applications in clean energy, gas storage and seperation, biomedical imaging, thin film devices, and catalysis? There are three ways for MOFs to use in catalysis: open metal sites (OMS), functional organic sites (FOS), and used as supports. In this thesis, we conducted our catalytic experiments according to the first and last ways. We constmcted two complexes using N, N\ 3,5-Benzenetriyltris (carbonylimino)] trisbenzoic acid (H3L) and manganous acetate [(CH3COO)2Mn], and these two complexes are used in knoevenagel reaction as OMS. And as supports, MIL-120 has been used to support nickel as active sites to catalyze the reduction of benzene.1. Two MOFs materials have been synthesized based on (CHsCOO)2Mn-4H2O and N, N\ N^-[l, 3, 5-Benzenetriyltris (carbonylimino)] trisbenzoic acid (H3L) under hydrothermal condition. And ancillary ligands have been used to design the different structure of MOFs rationally? The addition of 2, 2'-bipyridine (bpy) leaded to the ID crystal [Mn(L)(bpy)] (1), and the use of 1, T-( 1,4-butanediyl)bis(imidazole) (bbi) resulted in the 2D crystal [Mn(L)0.5(bbi)2.5(H2O)] (2). These two crystalline complexes have used to catalyze the knoevenagel reaction. It's demonstrated that 1 with ID structure showed better catalytic activity than 2 with 2D sructure?2. Under hydrothermal condition, aluminum nitrate [A1(NC)3)3?9H2O] and pyromellitic acid (1,2,4,5-benzenetetracarboxylic acid) have been used to seli-assemble MIL-120 with high thermal stability. And it's used to support nickel through impregnation method to obtain reduction catalysts, x-NM, which is used to catalyze the reduction reaction of benzene? It's shown that the catalyst 15-NM withKey Words:15% loa
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mn mofs nimil 120 合成 及其 催化 性能 研究
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