Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation
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] cat...
| Main Authors: | , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
American Chemical Society (ACS)
2017
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| Online Access: | http://hdl.handle.net/1721.1/109533 https://orcid.org/0000-0002-4347-0139 |
| Summary: | 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. |
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