Size‐Dependent Dispersion of Rhodium Clusters into Isolated Single Atoms at Low Temperature and the Consequences for CO Oxidation Activity

Albrahim, Malik A.; Shrotri, Abhijit; Unocic, Raymond R.; Hoffman, Adam S.; Bare, Simon R.; Karim, Ayman M.

doi:10.1002/ange.202308002

Title: Size‐Dependent Dispersion of Rhodium Clusters into Isolated Single Atoms at Low Temperature and the Consequences for CO Oxidation Activity

Journal Article · Tue Sep 19 00:00:00 EDT 2023 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202308002· OSTI ID:2001015

Albrahim, Malik A. ^[1]; Shrotri, Abhijit ^[2]; Unocic, Raymond R. ^[3]; Hoffman, Adam S. ^[4]; Bare, Simon R. ^[4];

^[1]

Department of Chemical Engineering Virginia Polytechnic Institute and State University Blacksburg Virginia 24060 USA
Institute for Catalysis Hokkaido University Kita ku, Sapporo Hokkaido 001-0021 Japan
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge Tennessee 37830 USA
Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park California 94025 USA

Abstract Understanding the dynamic structural evolution of supported metal clusters under reaction conditions is crucial to develop structure reactivity relations. Here, we followed the structure of different size Rh clusters supported on Al ₂ O ₃ using in situ/operando spectroscopy and ex situ aberration‐corrected electron microscopy. We report a dynamic evolution of rhodium clusters into thermally stable isolated single atoms upon exposure to oxygen and during CO oxidation. Rh clusters partially disperse into single atoms at room temperature and the extent of dispersion increases as the Rh size decreases and as the reaction temperature increases. A strong correlation is found between the extent of dispersion and the CO oxidation kinetics. More importantly, dispersing Rh clusters into single atoms increases the activity at room temperature by more than two orders of magnitude due to the much lower activation energy on single atoms (40 vs. 130 kJ/mol). This work demonstrates that the structure and reactivity of small Rh clusters are very sensitive to the reaction environment.

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Sponsoring Organization:: USDOE

OSTI ID:: 2001015

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 135 Journal Issue: 44; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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