Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation
Name
Elucidating the with SI.pdf
Size
2.01 MB
Format
Adobe PDF
Checksum (MD5)
80d02ff2dba3ffe4e8610c5b3a7f54f4
Author(s)
Bugnet, Matthieu
Botton, Gianluigi A.
Elias, Joseph Spanjaard
Artrith, Nongnuch
Giordano, Livia
Kolpak, Alexie M.
Shao-Horn, Yang
Date Issued
February 2016
Journal
ACS Catalysis
Publisher
American Chemical Society (ACS)
Citation
Elias, Joseph S., Nongnuch Artrith, Matthieu Bugnet, Livia Giordano, Gianluigi A. Botton, Alexie M. Kolpak, and Yang Shao-Horn. “Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation.” ACS Catalysis 6, no. 3 (March 4, 2016): 1675–1679.
Version
Author's final manuscript
Abstract
The active phase responsible for low-temperature CO oxidation in nanoparticulate CuO/CeO[subscript 2] catalysts was identified as surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x]. Contrary to previous studies, our measurements on a library of well-defined CuO/CeO[subscript 2] catalysts have proven that the CuO phase is a spectator species, whereas the surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] phase is active for CO oxidation. Using in situ X-ray absorption spectroscopy, we found that the copper ions in Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] remain at high oxidation states (Cu[superscript 3+] and Cu[superscript 2+]) under oxygen-rich catalytic conditions without any evidence for Cu+. Artificial neural network potential Monte Carlo simulations suggest that Cu[superscript 3+] and Cu[superscript 2+] preferentially segregate to the {100} surface of the Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] nanoparticle, which is supported by aberration-corrected electron microscopy measurements. These results pave the way for understanding, at the atomic level, the mechanisms and descriptors pertinent for CO oxidation on these materials and hence the rational design of next-generation catalysts.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Mechanical Engineering
Massachusetts Institute of Technology. Research Laboratory of Electronics
Terms of Use
Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/acscatal.5b02666
