Faculty Awards for Women: Catalytic Hydrogenitrogenation of Petroleum Derivatives

该研究计划将重点研究硫化和未硫化的Ni-Mo催化剂上的加氢脱氮反应中涉及的催化现象。本研究中使用的催化剂将通过三种不同的技术合成，即均相硫化物沉淀法、浸渍硫代盐分解法以及镍和钼离子在粘土基质中的插层。催化剂的表征将使用各种技术，包括BET比表面积和孔径分布分析、X射线衍射、扫描和透射电子显微镜、能量色散X射线分析、激光拉曼光谱和拉曼微探针和X射线光电子能谱。热分析技术还将通过程序升温还原、解吸和硫化研究来使用。除了催化剂的环境表征外，还将使用激光拉曼光谱仪和专门设计的原位拉曼池进行原位表征技术。将现场考察催化剂在氧化、还原、硫化、反应和失活过程中发生的变化。这些研究将被用来研究催化剂的活性形式和催化剂载体相互作用的性质。除了考察反应网络外，还将考察氢分压、反应温度和压力等反应参数的影响以及取代基的影响。最后，同位素标记技术将与动力学研究和原位激光拉曼光谱研究相结合，以深入了解加氢脱氮反应中涉及的催化现象。

The research program will focus on investigating the catalytic phenomena involved in hydrodenitrogenation reactions over sulfided and unsulfided Ni-Mo catalysts. The catalysts to be used in this study will be synthesized by three different techniques, namely, homogeneous sulfide precipitation, impregnated thiosalt decomposition and intercalation of nickel and molybdenum cations in clay matrices. Catalyst characterization will be performed using various techniques including BET surface area and pore size distribution analysis, X-ray diffraction, scanning and transmission electron microscopy, energy dispersive X-ray analysis, laser Raman Spectroscopy and Raman microprobe and X-ray photoelectron spectroscopy. Thermal analysis techniques will also be used through temperature-programmed reduction, desorption and sulfidation studies. In addition to ambient characterization of the catalysts, in-situ characterization techniques will also be adopted using a laser Raman spectrometer and a specially designed in-situ Raman cell. The changes that take place in the catalyst during oxidation, reduction, sulfidation, reaction and deactivation processes will be examined in-situ. These studies will be used to investigate the nature of the active form of the catalyst and the catalyst support interactions. In addition to examining the reaction network, the effect of reaction parameters such as hydrogen partial pressure, reaction temperature and pressure and the effect of substituents will also be investigated. Finally, isotopic labelling techniques will be combined with kinetic studies and in-situ laser Raman spectroscopy studies to gain insight into the catalytic phenomena involved in hydrodenitrogenation reactions.