期刊
CHINESE JOURNAL OF CATALYSIS
卷 42, 期 11, 页码 2078-2087出版社
ELSEVIER
DOI: 10.1016/S1872-2067(21)63884-6
关键词
FER-type zeolite; Aluminum siting; Structural characterization; Bronsted acid site; DME carbonylation
资金
- National Natural Science Foundation of China [21972136, 22008229, 21773233, 21991091, U20A20120]
- CAS Pioneer Hundred Talents Program [Y706071202]
- Dalian National Laboratory for Clean Energy Cooperation Fund, Chinese Academy of Sciences [DNL201908]
- Liaoning Revitalization Talents Program [XLYC1908010, XLYC1901006]
- BP Energy Innovation Laboratory
- STOE
By conducting Rietveld refinement against powder X-ray diffraction data, this study unraveled the constrained Al crystallographic sites in FER-type zeolites, revealing distinct local environments and Al-rich positions, which can explain the limited catalytic activity in certain reactions.
Crystallographic sites of Bronsted acids (Si-OH-Al) in zeolites, which are closely associated with the Al sites, play a significant and unique role in the catalytic application, especially when they are distributed in open channel systems or confined in cavities with small pore openings. In this article, we unraveled constrained Al crystallographic sites in FER-type zeolites containing the distinct local environments (10-ring channels and ferrierite cavities) by Rietveld refinement against the powder X-ray diffraction data. Final refinement demonstrates that regardless of the types of structure-directing agents and synthetic medium utilized, T1 and/or T3 are Al-rich positions, which are further confirmed by theoretical calculations. This new finding of constrained Al sites in the FER-type zeolite can well explain its limited catalytic activity in the DME carbonylation reaction. (C) 2021, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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