期刊
JOURNAL OF CATALYSIS
卷 314, 期 -, 页码 10-20出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2014.03.006
关键词
SSZ-13; Ethene-to-propene conversion; Framework dealumination; Bronsted acid sites; Naphthalene-based carbenium ions
资金
- National Natural Science Foundation of China [21303089]
- China Postdoctoral Science Foundation
- Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
- Ministry of Education of China [NCET-11-0251, IRT13022]
- Deutsche Forschungsgemeinschaft
- 111 Project [B12015]
Several types of microporous molecular sieves with similar n(Si)/n(Al) ratios (except for SAPO-34) and different pore structures were prepared and applied as ethene-to-propene (ETP) catalysts. H-SSZ-13 zeolite consisting of chabazite cages connected via 8-ring windows possessed the highest adsorption capacity for ethene and exhibited the best activity in the ETP conversion. The decreasing amount of Brensted acid sites after dealumination of H-SSZ-13 caused a prolonged lifetime of the catalyst in the ETP reaction. The reaction mechanism and deactivation behavior of H-SSZ-13 catalysts during the ETP process were investigated by in situ FT-IR, UV/Vis, GC-MS, TGA and H-1 MAS NMR methods. Ethene was rapidly oligomerized and converted into naphthalene-based carbenium ions, playing a significant role in the ETP reaction. The accumulation of these species lead to the formation of polycyclic aromatics, which are responsible for a total blocking of H-SSZ-13 pores, and cause the deactivation of the catalyst. (c) 2014 Elsevier Inc. All rights reserved.
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