Summary: | 博士 === 國立臺灣大學 === 化學研究所 === 102 === In view of the stringent global regulation and increasing R&;D demands in NOx removal (DeNOx), this thesis focuses on synthesis, characterization, and applications of Fe-based H-ZSM-5 zeolite catalysts for selective catalytic reduction (SCR) of NO by NH3. This thesis mainly consists of five chapters: Chapter 1 provides an overview and the chemistry, strategy, mechanism, and solid acid catalysts involved in a DeNOx process. Chapter 2 contains experimental details, including catalyst preparation methods, characterization techniques, and experimental procedures invoked during this study. Chapter 3 compares the SCR performances of mono- and bi-metallic Fe-based ZSM-5 catalysts prepared by different methods. Chapter 4 describes the syntheses and SCR performances of Lanthanide metal (Ce, Pr, Nd, and Sm)-incorporated Fe-based ZSM-5 catalysts prepared by reflux method. Chapter 5 summarizes the effect of Si/Al ratio of zeolite support on SCR performances of CeFe-ZSM-5 catalysts prepared by impregnation method. The catalysts so prepared were characterized by a variety of analytical and spectroscopic techniques, such as ICP-MS, XRF, XRD, BET, FE-TEM, H2-TPR, XPS, EPR, NH3-TPD, Pyridine-FTIR, and solid-state 27Al and 31P MAS NMR. It is conclusive that bimetallic catalysts (such as CeFe-ZSM-5) normally exhibit higher NH3-SCR activity (> 94%) over the temperature range of 350-500 oCthan mono-metal catalysts (such as Fe-ZSM-5). The superior SCR activity observed for the bimetallic catalysts has been attributed, for the first time, to the synergistic effect of Bronsted acidity originated from the zeolite support and strong Lewis acidity induced by the incorporated metals.
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