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The Dynamic Structure of Au38(SR)24 Nanoclusters Supported on CeO2 upon Pretreatment and CO Oxidation.


ABSTRACT: Atomically precise thiolate protected Au nanoclusters Au38(SC2H4Ph)24 on CeO2 were used for in-situ (operando) extended X-ray absorption fine structure/diffuse reflectance infrared fourier transform spectroscopy and ex situ scanning transmission electron microscopy-high-angle annular dark-field imaging/X-ray photoelectron spectroscopy studies monitoring cluster structure changes induced by activation (ligand removal) and CO oxidation. Oxidative pretreatment at 150 °C "collapsed" the clusters' ligand shell, oxidizing the hydrocarbon backbone, but the S remaining on Au acted as poison. Oxidation at 250 °C produced bare Au surfaces by removing S which migrated to the support (forming Au+-S), leading to highest activity. During reaction, structural changes occurred via CO-induced Au and O-induced S migration to the support. The results reveal the dynamics of nanocluster catalysts and the underlying cluster chemistry.

SUBMITTER: Pollitt S 

PROVIDER: S-EPMC7295362 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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The Dynamic Structure of Au<sub>38</sub>(SR)<sub>24</sub> Nanoclusters Supported on CeO<sub>2</sub> upon Pretreatment and CO Oxidation.

Pollitt Stephan S   Truttmann Vera V   Haunold Thomas T   Garcia Clara C   Olszewski Wojciech W   Llorca Jordi J   Barrabés Noelia N   Rupprechter Günther G  

ACS catalysis 20200508 11


Atomically precise thiolate protected Au nanoclusters Au<sub>38</sub>(SC<sub>2</sub>H<sub>4</sub>Ph)<sub>24</sub> on CeO<sub>2</sub> were used for in-situ (operando) extended X-ray absorption fine structure/diffuse reflectance infrared fourier transform spectroscopy and ex situ scanning transmission electron microscopy-high-angle annular dark-field imaging/X-ray photoelectron spectroscopy studies monitoring cluster structure changes induced by activation (ligand removal) and CO oxidation. Oxidat  ...[more]

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