Incorporation of Transition-Metal Complexes in Functionalized Mesoporous Silica and Their Activity toward the Oxidation of Aromatic Amines
Incorporation of Transition-Metal Complexes in Functionalized Mesoporous Silica and Their Activity toward the Oxidation of Aromatic Amines
复制标题
过渡金属配合物在功能化介孔二氧化硅中的掺入及其对芳香胺氧化的活性
DOI：
10.1021/jp000564p
复制
发表时间：
2000
影响因子：
3.3
通讯作者：
S. El‐Safty
中科院分区：
文献类型：
--
作者：
J. Evans;A. Zaki;M. El;S. El‐Safty
采用高浓度的非离子表面活性剂，在室温和低pH条件下制备了高度有序的介孔材料HISiO 2，得到六方有序相，孔径约为3.5 nm。接枝的氨基配体通过硅烷化过程共价键合到HISiO 2的内部孔表面。由此，固定化的过渡金属-水络合物如MnII-水（I）、CuII-水（II）、CoII-水（III）和ZnII-水（IV）配位到负载壁而不浸渍在表面上。漫反射光谱（DRS）和电子顺磁共振（EPR）的研究观察到，一定比例的MnII复合物被氧化到更高的氧化态，特别是MnIV。研究了邻氨基苯酚、邻苯二胺和对苯二胺与过渡金属-水-丙胺配合物之间的氧化还原反应动力学和机理。胺的氧化产物已通过紫外维斯光谱监测。The reac.
The highly ordered mesoporous material HISiO2 was prepared at room temperature and low pH utilizing a high concentration of nonionic surfactant to achieve a hexagonal ordered phase with a pore size of ∼3.5 nm. The grafted amino ligand was covalently bonded to the internal pore surface of HISiO2 through a silanation procedure. Thereby, immobilized transition-metal−aquo complexes such as MnII-aquo (I), CuII-aquo (II), CoII-aquo (III), and ZnII-aquo (IV) were coordinated to the supported wall without impregnation on the surface. Diffuse reflectance spectroscopy (DRS) and electron paramagnetic resonance (EPR) studies observed that a proportion of the MnII complex was oxidized to a higher oxidation state, particularly MnIV. The kinetics and mechanism of redox reactions between o-aminophenol, o-phenylenediamine, and p-pheneylenediamine and the incorporated transition-metal−aquo−propylamine complexes have been investigated. The oxidation products of the amines have been monitored by UV−vis spectroscopy. The reac...