In:
Angewandte Chemie, Wiley, Vol. 130, No. 17 ( 2018-04-16), p. 4732-4736
Abstract:
The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd 1 /CeO 2 ) and hexapalladium cluster–cerium oxide (Pd 6 /CeO 2 ), as confirmed by spherical‐aberration‐corrected transmission electron microscopy and X‐ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd 1 /CeO 2 shows extremely high catalytic activity with a TOF of 6739 h −1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd 6 /CeO 2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd 6 clusters hinder the interactions between hydroxy groups and the CeO 2 surface, thus suppressing synergy of Pd‐Ce perimeter.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v130.17
DOI:
10.1002/ange.201801103
Language:
English
Publisher:
Wiley
Publication Date:
2018
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1479266-7
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