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

TitleTransfer hydrogenation over sodium-modified ceria: Enrichment of redox sites active for alcohol dehydrogenation
Publication TypeJournal Article
Year of Publication2017
AuthorsNelson, NC, Boote, BW, Naik, P, Rossini, AJ, Smith, EA, Slowing, II
JournalJournal of Catalysis
Volume346
Pagination180-187
Date Published02
Type of ArticleArticle
ISBN Number0021-9517
Accession NumberWOS:000394195100019
KeywordsAlcohol dehydrogenation, ceo2 nanocrystals, Ceria, chemistry, co oxidation, Defect sites, defined surface planes, electronic-structure, Engineering, Flow chemistry, oxidation, oxygen vacancy, probing defect, ray photoelectron-spectroscopy, Redox, selective hydrogenation, sites, sodium, structure dependence, Transfer hydrogenation, x-ray
Abstract

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 (6x) 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. Thus, the difference in catalytic activity was attributed to the different numbers of 2-propanol adsorption and redox active sites on each catalyst. Published by Elsevier Inc.

DOI10.1016/j.jcat.2016.12.018
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3D Catalysis

Short TitleJ. Catal.
Alternate JournalJ. Catal.