Journal
ACS CATALYSIS
Volume 4, Issue 2, Pages 585-592Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs400908h
Keywords
ceria; cerium; XANES; ethanol; solvothermal; nanoparticles
Categories
Funding
- U.S. Department of Energy [DE-FG36-05GO15033]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-ACO2-06CH11357]
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Reducibility of ceria under steam reforming conditions and the effect of particle size on its reducibility was examined using two ceria samples with distinctly different mean particle sizes (3.5 nm versus 120 nm), but with similar polyhedral morphologies. The degree of reduction from Ce4+ to Ce3+ was characterized by temperature programmed reduction (TPR) and in situ X-ray absorption near edge structure spectroscopy (XANES) where the nanopolyhedra were observed to reduce much more readily compared to the larger particle-size sample. There was also significant reduction of the nanopolyhedra under ethanol steam reforming conditions. Ceria nanopolyhedra exhibited significantly more Ce3+ sites which contributed to a lower occurrence of surface acidic sites. The acidic/basic sites were probed by probe molecules such as pyridine and CO2 through in situ diffuse reflectance infrared spectroscopy (DRIFTS). The particle size also showed major differences in the steam reforming activity of ceria, with nanopolyhedra with a 3.5-nm mean particle size exhibiting significantly higher carbon cleavage and ethanol dehydration activity than its counterpart of 120 nm mean particle size.
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