CAREER: Synthesis, Characterization and Catalytic Evaluation of Novel Dealuminated Zeolite-based Catalysts for the Alkylation of i-Butane with 2-Butene

点击翻译按钮获取中文摘要

ABSTRACT Proposal Title: Synthesis, Characterization and Catalytic Evaluation of Novel Dealumination Zeolite-based Catalysts for the Alkylation of i-Butane with 2-Butene. Proposal Number: CTS-9702081 Principal Investigator: Panagiotis Smirniotis Institution: Univ. of Cincinnati Dealuminated ZSM-12, a large-pore, one-dimensional, high-silica, 12-member ring zeolite, will be studied for the alkylation of i-butane with 2-butene. High stability is expected as a consequence of low coking formation, and it is the goal of this research to understand the coking mechanism and the zeolite features leading to stability. Dealumination of structurally selected Al will be studied as a means to improve anti-coking behavior. For this purpose, zeolite L, which contains long channels connecting large cavities, will be utilized. Selective dealumination of Al at channel-to-cavity connections will be effected by the dimer of 5-bromomethyl-m-phthalic acid produced inside the zeolite cavity. The dimerization will be initiated by a suitable radical initiator. Characterization of the zeolite will involve X-ray diffraction, 27Al NMR to distinguish framework from non-framework Al, SEM, infrared spectroscopy of adsorbed bases to determine Bronsted and Lewis acidity, XPS to distinguish types of framework Al, ammonia TPD to measure their acidity, and EXAFS to investigate Al coordination and location. The removal of Al from channel-cavity intersections in zeolite L will be assessed with cyclopentane isomerization. The coking mechanism will be studied by gravimetry and by mass spectrometry of soluble coke, and the alkylation mechanisms will be studied kinetically. The research is significant to the fuel industry and leads to environmentally benign processes.