Transfer hydrogenation over sodium-modified ceria: Enrichment of redox sites active for alcohol dehydrogenation

Journal Article · Tue Jan 17 00:00:00 EST 2017 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2016.12.018· OSTI ID:1347411

Nelson, Nicholas C. ^[1]; Boote, Brett W. ^[1]; Naik, Pranjali ^[1]; Rossini, Aaron J. ^[1]; Smith, Emily A. ^[1]; Slowing, Igor I. ^[1]

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1. Ames Lab. and Iowa State Univ., Ames, IA (United States)

Ceria (CeO₂) and sodium-modified ceria (Ce-Na) were prepared through combustion synthesis. Palladium was deposited onto the supports (Pd/CeO₂ and Pd/Ce-Na) and their activity for the aqueous-phase transfer hydrogenation of phenol using 2-propanol under liquid flow conditions was studied. Pd/Ce-Na showed a marked increase (6×) in transfer hydrogenation activity over Pd/CeO₂. Material characterization indicated that water-stable sodium species were not doped into the ceria lattice, but rather existed as subsurface carbonates. Modification of ceria by sodium provided more adsorption and redox active sites (i.e. defects) for 2-propanol dehydrogenation. This effect was an intrinsic property of the Ce-Na support and independent of Pd. The redox sites active for 2-propanol dehydrogenation were thermodynamically equivalent on both supports/catalysts. At high phenol concentrations, the reaction was limited by 2-propanol adsorption. Furthermore, the difference in catalytic activity was attributed to the different numbers of 2-propanol adsorption and redox active sites on each catalyst.

• Research Organization: Ames Lab., Ames, IA (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• Grant/Contract Number: AC02-07CH11358
• OSTI ID: 1347411
• Alternate ID(s): OSTI ID: 1350060; OSTI ID: 1420008
• Report Number(s): IS-J-9166; IS-J-9026; PII: S0021951716303323
• Journal Information: Journal of Catalysis, Vol. 346, Issue C; ISSN 0021-9517
• Publisher: Elsevier
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
transfer hydrogenation
ceria
sodium
alcohol dehydrogenation
redox
defect sites
oxidation
flow chemistry