Investigation of the Physical, Chemical, and Catalytic Properties of Transition Metal Cations in Zeolites

摘要-贝尔-9713143名教授。亚历克西斯·T·贝尔和杰弗里·A·赖默将研究过渡金属阳离子交换沸石的催化、结构和稳定性。测试反应将包括N2O分解和烯烃二聚。物理化学探针将包括TPD、红外光谱、拉曼光谱、核磁共振光谱、ESR光谱和紫外可见光谱，以确定反应前后阳离子的分布和氧化状态，以及反应过程中吸附和反应中间体的同一性。还将使用其他技术，如用于微观结构的X射线衍射和扫描电子显微镜，以及用于磁化率的古伊天平。将利用双共振、谱线展宽和魔角旋转核磁共振技术来探索交换阳离子的分布和电子性质。将确定沸石结构、硅铝比、共交换阳离子、阳离子负载量以及合成和反应条件对催化、结构和稳定性的影响。特别是，这项研究将涉及使用硅铝比高于10的商用ZMS-5，与例如铜、钴、银、镓、铟和锌进行阳离子交换。研究过渡金属阳离子交换沸石的合成-结构-性能-性能关系，为过渡金属阳离子交换沸石的设计和工业应用提供依据。这种类型的催化剂在石油、大宗化工、精细化工和环保行业中具有重要意义。

Abstract - Bell - 9713143 Profs. Alexis T. Bell and Jeffrey A. Reimer will study the catalytic, structural and stability properties of transition-metal cation-exchanged zeolites. Test reactions will include N2O decomposition and olefin dimerization. The physico-chemical probes will involve TPD, and infrared, Raman, NMR, ESR, and UV-Vis spectroscopy, both ex situ and in situ, in order to determine cation distribution and oxidation state before and after reaction, and adsorbed and reactive intermediates identity during reaction. Other techniques such as XRD and SEM for microstructure, and Guoy balance for magnetic susceptibility, will also be used. Double resonance, line broadening, and magic-angle spinning NMR techniques will be exploited to probe the distribution and electronic properties of exchanged cations. The influence of zeolite structure, Si/Al ratio, co-exchanged cations, cation loading, and synthesis and reaction conditions, on catalytic, structural, and stability properties will be determined. In particular, the study will involve the use of commercial ZMS-5 with Si/Al ratios above 10, cation-exchanged with, e.g., Cu, Co, Ag, Ga, In, and Zn. The synthesis-structure-property-performance relations will be studied to provide a basis for the design and industrial application of transition-metal cation-exchanged zeolites. This type of catalysts is of relevance in the petroleum, bulk chemical, fine chemical and environmental protection industries.