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Kwak, Ja Hun
Molecular Catalysis Lab.
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Surface Density Dependent Catalytic Activity of Single Palladium Atoms Supported on Ceria**

Author(s)
Kim, YongseonCollinge, GregLee, Mal-SoonKhivantsev, KonstantinCho, Sung JuneGlezakou, Vassiliki-AlexandraRousseau, RogerSzanyi, JanosKwak, Ja Hun
Issued Date
2021-10
DOI
10.1002/anie.202105750
URI
https://scholarworks.unist.ac.kr/handle/201301/53424
Fulltext
https://onlinelibrary.wiley.com/doi/10.1002/anie.202105750
Citation
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, v.60, no.42, pp.22769 - 22775
Abstract
The analogy between single-atom catalysts (SACs) and molecular catalysts predicts that the specific catalytic activity of these systems is constant. We provide evidence that this prediction is not necessarily true. As a case in point, we show that the specific activity over ceria-supported single Pd atoms linearly increases with metal atom density, originating from the cumulative enhancement of CeO2 reducibility. The long-range electrostatic footprints (approximate to 1.5 nm) around each Pd site overlap with each other as surface Pd density increases, resulting in an observed deviation from constant specific activity. These cooperative effects exhaust previously active O atoms above a certain Pd density, leading to their permanent removal and a consequent drop in reaction rate. The findings of our combined experimental and computational study show that the specific catalytic activity of reducible oxide-supported single-atom catalysts can be tuned by varying the surface density of single metal atoms.
Publisher
WILEY-V C H VERLAG GMBH
ISSN
1433-7851
Keyword (Author)
CO oxidationelectrostatic effectsPdCeO2reducible oxide supports
Keyword
CO OXIDATIONSTRUCTURAL-PROPERTIESCEO2 NANOCRYSTALSCARBON-MONOXIDESITESALUMINANANOPARTICLESOXYGENWATER

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