Elucidating the active phases of CoOx films on Au(111) in the CO oxidation reaction

Hao Chen, Lorenz J. Falling, Heath Kersell, George Yan, Xiao Zhao, Judit Oliver-Meseguer, Max Jaugstetter, Slavomir Nemsak, Adrian Hunt, Iradwikanari Waluyo, Hirohito Ogasawara, Alexis T. Bell, Philippe Sautet and Miquel Salmeron ()
Additional contact information
Hao Chen: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Lorenz J. Falling: Lawrence Berkeley National Laboratory
Heath Kersell: Lawrence Berkeley National Laboratory
George Yan: University of California, Los Angeles
Xiao Zhao: Lawrence Berkeley National Laboratory
Judit Oliver-Meseguer: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Max Jaugstetter: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Slavomir Nemsak: Lawrence Berkeley National Laboratory
Adrian Hunt: Brookhaven National Laboratory
Iradwikanari Waluyo: Brookhaven National Laboratory
Hirohito Ogasawara: SLAC National Accelerator Laboratory
Alexis T. Bell: Chemical Sciences Division, Lawrence Berkeley National Laboratory
Philippe Sautet: University of California, Los Angeles
Miquel Salmeron: Lawrence Berkeley National Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Noble metals supported on reducible oxides, like CoOx and TiOx, exhibit superior activity in many chemical reactions, but the origin of the increased activity is not well understood. To answer this question we studied thin films of CoOx supported on an Au(111) single crystal surface as a model for the CO oxidation reaction. We show that three reaction regimes exist in response to chemical and topographic restructuring of the CoOx catalyst as a function of reactant gas phase CO/O2 stoichiometry and temperature. Under oxygen-lean conditions and moderate temperatures (≤150 °C), partially oxidized films (CoOx 1) forms containing Co3+ species that are effective in a wide temperature range. Resonant photoemission spectroscopy (ResPES) revealed the unique role of Co3+ sites in catalyzing the CO oxidation. Density function theory (DFT) calculations provided deeper insights into the pathway and free energy barriers for the reactions on these oxide phases. These findings in this work highlight the versatility of catalysts and their evolution to form different active phases, both topological and chemically, in response to reaction conditions exposing a new paradigm in the catalyst structure during operation.

Date: 2023
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DOI: 10.1038/s41467-023-42301-7

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