Zeolite Encaged Transition Metal-Proton Adducts Catalytic, Selectivity and Dispersion Stability

[221841] Wolfgang Sachtler这是一项关于沸石中金属-质子加合物的系统研究，包括这些加合物在改变金属的催化特性和将金属团簇锚定在沸石上的作用。一个需要解决的问题是，在含有质子的沸石中，过渡金属的催化活性增强是由于金属颗粒的电子缺乏还是由于加合质子在催化反应中的化学参与。这项工作的重点是铑簇，但也包括对钯和铂的额外工作。用光电子能谱法测定了金属和金属质子加合物上的碳氢化合物转化反应速率和金属的电子缺乏率。其他使用的表征技术包括x射线吸收法（使用同步辐射）、电子显微镜、红外光谱、核磁共振、温度程序质谱法和同位素交换。研究了醇类和胺类对金属在沸石中烧结的影响。所研究的沸石包括Y、L和ZSM-5。本文所研究的催化剂体系在石油炼制以及纤维和塑料工业的单体生产中具有重要意义。这里揭示的影响可能会极大地影响这些系统的性能或生命周期。

9221841 Wolfgang Sachtler This is a systematic study of metal-proton adducts in zeolites, including the role of these adducts in modifying the catalytic characteristics of metal and in anchoring metal clusters to the zeolite. One issue addressed is whether the enhanced catalytic activity of transition metals in proton-containing zeolites is due to the electron deficiency of the metal particles or to the chemical participation of adduct protons in the catalytic reaction. The emphasis in this effort is on rhodium clusters although additional work on palladium and platinum is also included. The rates of hydrocarbon conversion reactions on metals and metal- proton adducts are compared with the electron deficiency of the metals as determined by photoelectron spectroscopy. Other characterization techniques used include X-ray absorption methods (using synchrotron radiation), electron microscopy, infrared spectroscopy, nuclear magnetic resonance, temperature-programmed mass spectrometric methods, and isotopic exchange. The effects of alcohols and amines on metal sintering in zeolites is also study. Zeolites studied include Y, L, and ZSM-5. The catalyst systems under study here are important in petroleum refining and in the production of monomers for the fiber and plastics industries. The effects uncovered here could dramatically influence the performance or lifetimes of these systems.