期刊
JOURNAL OF CATALYSIS
卷 300, 期 -, 页码 251-259出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.01.011
关键词
Binuclear iron sites; Extra-framework Al; N2O decomposition; Fe/ZSM-35; Raman spectroscopy
资金
- Program Strategic Scientific Alliances between China and the Netherlands [2008DFB50130]
- National Basic Research Program of China (973 Program) [2009CB623507]
- National Natural Science Foundation of China (NSFC) [21003122]
The influence of extra-framework Al via AlCl3 deposition on the structure of the active Fe sites in Fe/ZSM-35 was investigated by Si-29 MAS NMR, UV-visible diffuse reflectance spectroscopy, infrared spectroscopy, UV Raman spectroscopy, and Fe-57 Mossbauer spectroscopy combined with catalytic decomposition of N2O. It is found that high-temperature treatment considerably modifies the iron speciation. UV-visible diffuse reflectance spectra and in situ infrared spectra of NO adsorption show that a significant amount of clustered and cationic Fe species is transformed into extra-framework Fe-O-Al mixed oxide species by high-temperature treatment. UV Raman spectra and Fe-57 Mossbauer spectra suggest the generation of a binuclear Fe site stabilized by extra-framework Al species with a feature Raman band at 875 cm(-1), which is associated with the high activity of N2O decomposition. A possible explanation is that the addition of extra-framework Al species is beneficial for the formation of binuclear active Fe sites bound to extra-framework Al. (C) 2013 Published by Elsevier Inc.
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