期刊
JOURNAL OF CATALYSIS
卷 391, 期 -, 页码 11-24出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2020.07.035
关键词
Metal clusters; Isolated atoms; Pt; MFI zeolite; Propane dehydrogenation; Structural evolution
资金
- European Union through the European Research Council [ERC-AdG-2014-671093]
- Spanish government through the Severo Ochoa Program [SEV-2016-0683]
- FEDER/MINECO [MAT2017-87579-R, MAT2016-81118-P]
- CAPES (Science without Frontiers) [13191/13-6]
- ExxonMobil
To achieve high-loading of stable subnanometric metal clusters on solid carriers is a challenge since those small metal clusters have strong tendency to sinter into larger nanoparticles. Development of facile synthesis methodologies to obtain subnanometric metal catalysts with high metal loading and high stability against sintering at high temperature (>500 degrees C) in reductive atmosphere (such as H-2) is critical for the practical applications. In this work, we will present and discuss the generation of high-loading (similar to 1.4 wt%) subnanometric Pt clusters confined in the sinusoidal channels of MFI zeolite, on the basis of the atomic-level understanding on the evolution of Pt and Sn species during high-temperature oxidation-reduction treatments. It will be shown that the structural evolution of Pt and Sn species is dependent on the post-synthesis treatments. The Pt particles on the external surface can disintegrate into subnanometric Pt species and get stabilized in the zeolite channels during high-temperature calcination in air while Sn species migrate from surface region to internal region during high-temperature reduction treatment at 650 degrees C. The resultant material containing bimetallic PtSn clusters confined in the 10MR sinusoidal channels of the purely siliceous MFI zeolite show excellent catalytic activity and stability, as demonstrated for dehydrogenation of light alkanes at high reaction temperature. (C) 2020 Elsevier Inc. All rights reserved.
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