期刊
SCIENCE CHINA-CHEMISTRY
卷 64, 期 7, 页码 1103-1110出版社
SCIENCE PRESS
DOI: 10.1007/s11426-020-9867-x
关键词
Cu; CeO(2)catalysts; ceria shape; copper-ceria interface; atomically dispersed copper sites; monolayers; low-temperature water-gas shift reaction
资金
- National Natural Science Foundation of China [21761132031, 21533009]
The density of surface oxygen vacancies induced by the shape of ceria determines the structure and chemical state of copper species. Copper atoms can be atomically dispersed on ceria particles and rods, but form clusters on cubic ceria. The active sites for the water-gas shift reaction can be tuned by dispersing Cu species on shape-controlled ceria particles.
The structure of copper species, dispersed on nanostructured ceria (particles, rods and cubes), was analyzed by scanning transmission electron microscopy (STEM) and X-ray photoelectron spectroscopy (XPS). It was interestingly found that the density of surface oxygen vacancies (or defect sites), induced by the shape of ceria, determined the geometrical structure and the chemical state of copper species. Atomically dispersed species and monolayers containing few to tens of atoms were formed on ceria particles and rods owing to the enriched anchoring sites, but copper clusters/particles co-existed, together with the highly dispersed atoms and monolayers, on cubic ceria. The atomically dispersed copper sites and monolayers interacted strongly with ceria, involving a remarkable charge transfer from copper to ceria at their interfaces. The activity for the low-temperature water-gas shift reaction of the Cu/CeO(2)catalysts was associated with the fraction of the positively-charged copper atoms, demonstrating that the active sites could be tuned by dispersing Cu species on shape-controlled ceria particles.
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