期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 54, 期 48, 页码 14270-14275出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201506045
关键词
catalysis; ceria; hydrogenation; NMR spectroscopy; nuclear spin hyperpolarization
资金
- ACS-PRF [52258-ND5]
- NSF [CHE-1507230]
- University of Florida
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1507230] Funding Source: National Science Foundation
Intense para-hydrogen-enhanced NMR signals are observed in the hydrogenation of propene and propyne over ceria nanocubes, nano-octahedra, and nanorods. The well-defined ceria shapes, synthesized by a hydrothermal method, expose different crystalline facets with various oxygen vacancy densities, which are known to play a role in hydrogenation and oxidation catalysis. While the catalytic activity of the hydrogenation of propene over ceria is strongly facet-dependent, the pairwise selectivity is low (2.4% at 375 degrees C), which is consistent with stepwise H atom transfer, and it is the same for all three nanocrystal shapes. Selective semi-hydrogenation of propyne over ceria nanocubes yields hyperpolarized propene with a similar pairwise selectivity of (2.7% at 300 degrees C), indicating product formation predominantly by a non-pairwise addition. Ceria is also shown to be an efficient pairwise replacement catalyst for propene.
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