期刊
JOURNAL OF CATALYSIS
卷 338, 期 -, 页码 340-348出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2016.02.032
关键词
Hollow titanium silicalite; Irreversible deactivation; Cyclohexanone ammoximation; Amorphous TiO2-SiO2 oxide; H2O2 decomposition
资金
- State Basic Research Project 973 by the Ministry of Science and Technology of People's Republic of China [2006CB202508]
- China Petrochemical Corporation (SINOPEC Group)
- Swedish Research Council (VR)
- Swedish Governmental Agency for Innovation Systems (VINNOVA)
Commercial deactivated HTS zeolite has been investigated by multiple characterization methods and catalytic evaluations. These indicate that structural and textural properties are not mainly ascribed to the irreversible deactivation, but some framework Ti species are transformed into Ti-rich nanoparticles. Both Bronsted and Lewis acid sites are observed in deactivated HTS zeolite, which agrees well with the spectroscopic characterization results and Tanabe's acidity theory on mixed binary oxides. Hence the acidic Ti-rich aggregates are attributed to the amorphous TiO2-SiO2 nanoparticles located on the external surface of the zeolite. Furthermore, it is demonstrated that the catalytic performance of deactivated HTS zeolite in phenol hydroxylation is seriously dependent on its acidity properties, which can accelerate the decomposition of H2O2. As a consequence, we conclude that the irreversible deactivation of HTS zeolite in the ammoximation process is caused by the formation of acidic amorphous TiO2-SiO2 nanoparticles catalyzing the fast H2O2 decomposition reaction. (C) 2016 Elsevier Inc. All rights reserved.
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